I think it is a good approach to study some other instruction sets.
A small one would be the MSP430 from TI it is a 16bit Processor with about 22 instructions.
http://www.physics.mcmaster.ca/phys3b06/MSP430/MSP430_Instruction_Set_Summary.pdf
You could also look into the Atmel AVRs they have also a quite small instruction set.
In a little project of mine I tried to develop a simple 32 bit processor in VHDL with a small instruction set (14 instructions):
Due to my current free time it is not fully finished. The instructions are implemented but two are not tested and maybe some status flags are missing.