The spec sums it up very well. Section 5.5, "Atomicity of variable references":
Reads and writes of the following data types are atomic: bool, char,
  byte, sbyte, short, ushort, uint, int, float, and reference types. In
  addition, reads and writes of enum types with an underlying type in
  the previous list are also atomic. Reads and writes of other types,
  including long, ulong, double, and decimal, as well as user-defined
  types, are not guaranteed to be atomic. Aside from the library
  functions designed for that purpose, there is no guarantee of atomic
  read-modify-write, such as in the case of increment or decrement.
Conclusions:
- Independent reads/writes are atomic (but only for some data types)
 
- Read/modify/write (such as 
i++) is never atomic 
- You can use the 
Interlocked class methods to achieve atomicity when it's not already guaranteed 
In cases where Interlocked functionality is not enough there is no other option than to use a synchronization primitive, such as Monitor.Enter (which the compiler also exposes through the lock statement).