This is C# but the snippet shows what you are currently doing, and how to do it so that it works.
using System.Collections.Generic;
using System.Windows.Forms;
namespace DataGridNoBinding_47308996
{
    public partial class Form1 : Form
    {
        DataGridView dgv = new DataGridView();
        public Form1()
        {
            InitializeComponent();
            dgv.Dock = DockStyle.Fill;
            dgv.AutoGenerateColumns = false;
            dgv.Columns.Add("Key","Key");
            dgv.Columns.Add("Value", "Value");
            this.Controls.Add(dgv);
            Dictionary<string, string> dgvdata = new Dictionary<string, string>();
            for (int i = 0; i < 10; i++)
            {
                dgvdata.Add($"key{i}", $"value{i}");
            }
            //AddToGridNoWork(dgvdata);
            AddToGridDoesWork(dgvdata);
        }
        /// <summary>
        /// This method does not work. This emulates what you are currently doing.
        /// </summary>
        /// <param name="dgvdata"></param>
        private void AddToGridNoWork(Dictionary<string, string> dgvdata)
        {
            foreach (KeyValuePair<string, string> item in dgvdata)
            {
                dgv.Rows.Add();
                dgv.Rows[dgv.Rows.Count - 1].Cells[0].Value = item.Key;
                dgv.Rows[dgv.Rows.Count - 1].Cells[1].Value = item.Value;
                dgv.Refresh();
            }
        }
        /// <summary>
        /// This method does work.
        /// Add a new row to the Grid and store the new row index in rowindex
        /// Then use the variable rowindex to update the correct row
        /// </summary>
        /// <param name="dgvdata"></param>
        private void AddToGridDoesWork(Dictionary<string, string> dgvdata)
        {
            foreach (KeyValuePair<string, string> item in dgvdata)
            {
                int rowindex = dgv.Rows.Add();
                dgv.Rows[rowindex].Cells[0].Value = item.Key;
                dgv.Rows[rowindex].Cells[1].Value = item.Value;
            }
        }
    }
}
In your VB.net application, it's probably just a matter of doing somehting like this
dim newRowIndex as Integer
newRowIndex = DataGridView1.Rows.Add("")
For ix As Integer = 0 To 5
    DataGridView1.Rows(newRowIndex).Cells(ix).Value = words(ix)
Next
With DataDriver instead
Here's my code, re spun using a data driver instead of the StreamReader
using System;
using System.Collections.Generic;
using System.Windows.Forms;
using System.Data.OleDb;
using System.Data;
namespace DataGridNoBinding_47308996
{
    public partial class Form1 : Form
    {
        DataGridView dgv = new DataGridView();
        public Form1()
        {
            InitializeComponent();
            dgv.Dock = DockStyle.Fill;
            this.Controls.Add(dgv);
            Dictionary<string, string> dgvdata = new Dictionary<string, string>();
            for (int i = 0; i < 10; i++)
            {
                dgvdata.Add($"key{i}", $"value{i}");
            }
            //AddToGridNoWork(dgvdata);
            //AddToGridDoesWork(dgvdata);
            //AddToGridUsingDataDriver(@"M:\StackOverflowQuestionsAndAnswers\DataGridNoBinding_47308996\SampleData.csv");
            AddToGridByBindingTheWholeTable(@"M:\StackOverflowQuestionsAndAnswers\DataGridNoBinding_47308996\SampleData.csv");
        }
        /// <summary>
        /// This method will do what you want using a Data Driver instead of a StreamReader
        /// Though, this method binds the whole DataTable to the DataGridView instead of manually creating 1 row per data row
        /// </summary>
        /// <param name="dataFilePath"></param>
        private void AddToGridByBindingTheWholeTable(string dataFilePath)
        {
            dgv.AutoGenerateColumns = true;
            string connstring = $"Provider=Microsoft.ACE.OLEDB.12.0;Data Source={System.IO.Path.GetDirectoryName(dataFilePath)};Extended Properties=\"Text;HDR=NO;FMT=Delimited\"";
            OleDbConnection conn = new OleDbConnection(connstring);
            OleDbCommand command = new OleDbCommand($"select * from {System.IO.Path.GetFileName(dataFilePath)}", conn);
            OleDbDataAdapter dataAdapter = new OleDbDataAdapter(command);
            DataTable dt = new DataTable();
            conn.Open();
            dataAdapter.Fill(dt);
            conn.Close();
            dgv.DataSource = dt;
        }
        /// <summary>
        /// This method will do what you want using a Data Driver instead of a StreamReader
        /// In this method, we are actively creating 1 DataGridRow for each DataRow in the DataTable
        /// </summary>
        /// <param name="dataFilePath"></param>
        private void AddToGridUsingDataDriver(string dataFilePath)
        {
            dgv.AutoGenerateColumns = false;
            dgv.Columns.Add("Key", "Key");
            dgv.Columns.Add("Value", "Value");
            string connstring = $"Provider=Microsoft.ACE.OLEDB.12.0;Data Source={System.IO.Path.GetDirectoryName(dataFilePath)};Extended Properties=\"Text;HDR=NO;FMT=Delimited\"";
            OleDbConnection conn = new OleDbConnection(connstring);
            OleDbCommand command = new OleDbCommand($"select * from {System.IO.Path.GetFileName(dataFilePath)}", conn);
            OleDbDataAdapter dataAdapter = new OleDbDataAdapter(command);
            DataTable dt = new DataTable();
            conn.Open();
            dataAdapter.Fill(dt);
            conn.Close();
            if (dt != null && dt.Rows.Count > 0)
            {
                foreach (DataRow item in dt.Rows)
                {
                    int newrowid = dgv.Rows.Add();
                    dgv.Rows[newrowid].Cells[0].Value = item.Field<string>(0);
                    dgv.Rows[newrowid].Cells[1].Value = item.Field<string>(1);
                }
            }
            dgv.Refresh();
        }
        /// <summary>
        /// This method does not work. This emulates what you are currently doing.
        /// </summary>
        /// <param name="dgvdata"></param>
        private void AddToGridNoWork(Dictionary<string, string> dgvdata)
        {
            dgv.AutoGenerateColumns = false;
            dgv.Columns.Add("Key","Key");
            dgv.Columns.Add("Value", "Value");
            foreach (KeyValuePair<string, string> item in dgvdata)
            {
                dgv.Rows.Add();
                dgv.Rows[dgv.Rows.Count - 1].Cells[0].Value = item.Key;
                dgv.Rows[dgv.Rows.Count - 1].Cells[1].Value = item.Value;
                dgv.Refresh();
            }
        }
        /// <summary>
        /// This method does work.
        /// Add a new row to the Grid and store the new row index in rowindex
        /// Then use the variable rowindex to update the correct row
        /// </summary>
        /// <param name="dgvdata"></param>
        private void AddToGridDoesWork(Dictionary<string, string> dgvdata)
        {
            dgv.AutoGenerateColumns = false;
            dgv.Columns.Add("Key", "Key");
            dgv.Columns.Add("Value", "Value");
            foreach (KeyValuePair<string, string> item in dgvdata)
            {
                int rowindex = dgv.Rows.Add();
                dgv.Rows[rowindex].Cells[0].Value = item.Key;
                dgv.Rows[rowindex].Cells[1].Value = item.Value;
            }
        }
    }
}