Unaligned atomic memory operations on a processor using a load-store instruction set architecture (ISA) that requires aligned accesses are performed by widening the memory access to an aligned address by the next larger power of two (e.g., 4-byte access is widened to 8 bytes, and 8-byte access is widened to 16 bytes). Data processing operations supported by the load-store ISA including shift, rotate, and bitfield manipulation are utilized to modify only the bytes in the original unaligned address so that the atomic memory operations are aligned to the widened access address. The aligned atomic memory operations using the widened accesses avoid the faulting exceptions associated with unaligned access for most 4-byte and 8-byte accesses. Exception handling is performed in cases in which memory access spans a 16-byte boundary.