All answers are writing single bytes only - what if you want to fill a byte array with words? Or floats? I find use for that now and then. So after having written similar code to 'memset' in a non-generic way a few times and arriving at this page to find good code for single bytes, I went about writing the method below.
I think PInvoke and C++/CLI each have their drawbacks. And why not have the runtime 'PInvoke' for you into mscorxxx? Array.Copy and Buffer.BlockCopy are native code certainly. BlockCopy isn't even 'safe' - you can copy a long halfway over another, or over a DateTime as long as they're in arrays.
At least I wouldn't go file new C++ project for things like this - it's a waste of time almost certainly.
So here's basically an extended version of the solutions presented by Lucero and TowerOfBricks that can be used to memset longs, ints, etc as well as single bytes.
public static class MemsetExtensions
{
    static void MemsetPrivate(this byte[] buffer, byte[] value, int offset, int length) {
        var shift = 0;
        for (; shift < 32; shift++)
            if (value.Length == 1 << shift)
                break;
        if (shift == 32 || value.Length != 1 << shift)
            throw new ArgumentException(
                "The source array must have a length that is a power of two and be shorter than 4GB.", "value");
        int remainder;
        int count = Math.DivRem(length, value.Length, out remainder);
        var si = 0;
        var di = offset;
        int cx;
        if (count < 1) 
            cx = remainder;
        else 
            cx = value.Length;
        Buffer.BlockCopy(value, si, buffer, di, cx);
        if (cx == remainder)
            return;
        var cachetrash = Math.Max(12, shift); // 1 << 12 == 4096
        si = di;
        di += cx;
        var dx = offset + length;
        // doubling up to 1 << cachetrash bytes i.e. 2^12 or value.Length whichever is larger
        for (var al = shift; al <= cachetrash && di + (cx = 1 << al) < dx; al++) {
            Buffer.BlockCopy(buffer, si, buffer, di, cx);
            di += cx;
        }
        // cx bytes as long as it fits
        for (; di + cx <= dx; di += cx)
            Buffer.BlockCopy(buffer, si, buffer, di, cx);
        // tail part if less than cx bytes
        if (di < dx)
            Buffer.BlockCopy(buffer, si, buffer, di, dx - di);
    }
}
Having this you can simply add short methods to take the value type you need to memset with and call the private method, e.g. just find replace ulong in this method:
    public static void Memset(this byte[] buffer, ulong value, int offset, int count) {
        var sourceArray = BitConverter.GetBytes(value);
        MemsetPrivate(buffer, sourceArray, offset, sizeof(ulong) * count);
    }
Or go silly and do it with any type of struct (although the MemsetPrivate above only works for structs that marshal to a size that is a power of two):
    public static void Memset<T>(this byte[] buffer, T value, int offset, int count) where T : struct {
        var size = Marshal.SizeOf<T>();
        var ptr = Marshal.AllocHGlobal(size);
        var sourceArray = new byte[size];
        try {
            Marshal.StructureToPtr<T>(value, ptr, false);
            Marshal.Copy(ptr, sourceArray, 0, size);
        } finally {
            Marshal.FreeHGlobal(ptr);
        }
        MemsetPrivate(buffer, sourceArray, offset, count * size);
    }
I changed the initblk mentioned before to take ulongs to compare performance with my code and that silently fails - the code runs but the resulting buffer contains the least significant byte of the ulong only.
Nevertheless I compared the performance writing as big a buffer with for, initblk and my memset method. The times are in ms total over 100 repetitions writing 8 byte ulongs whatever how many times fit the buffer length. The for version is manually loop-unrolled for the 8 bytes of a single ulong.
Buffer Len  #repeat  For millisec  Initblk millisec   Memset millisec
0x00000008  100      For   0,0032  Initblk   0,0107   Memset   0,0052
0x00000010  100      For   0,0037  Initblk   0,0102   Memset   0,0039
0x00000020  100      For   0,0032  Initblk   0,0106   Memset   0,0050
0x00000040  100      For   0,0053  Initblk   0,0121   Memset   0,0106
0x00000080  100      For   0,0097  Initblk   0,0121   Memset   0,0091
0x00000100  100      For   0,0179  Initblk   0,0122   Memset   0,0102
0x00000200  100      For   0,0384  Initblk   0,0123   Memset   0,0126
0x00000400  100      For   0,0789  Initblk   0,0130   Memset   0,0189
0x00000800  100      For   0,1357  Initblk   0,0153   Memset   0,0170
0x00001000  100      For   0,2811  Initblk   0,0167   Memset   0,0221
0x00002000  100      For   0,5519  Initblk   0,0278   Memset   0,0274
0x00004000  100      For   1,1100  Initblk   0,0329   Memset   0,0383
0x00008000  100      For   2,2332  Initblk   0,0827   Memset   0,0864
0x00010000  100      For   4,4407  Initblk   0,1551   Memset   0,1602
0x00020000  100      For   9,1331  Initblk   0,2768   Memset   0,3044
0x00040000  100      For  18,2497  Initblk   0,5500   Memset   0,5901
0x00080000  100      For  35,8650  Initblk   1,1236   Memset   1,5762
0x00100000  100      For  71,6806  Initblk   2,2836   Memset   3,2323
0x00200000  100      For  77,8086  Initblk   2,1991   Memset   3,0144
0x00400000  100      For 131,2923  Initblk   4,7837   Memset   6,8505
0x00800000  100      For 263,2917  Initblk  16,1354   Memset  33,3719
I excluded the first call every time, since both initblk and memset take a hit of I believe it was about .22ms for the first call. Slightly surprising my code is faster for filling short buffers than initblk, seeing it got half a page full of setup code. 
If anybody feels like optimizing this, go ahead really. It's possible.