Litecoin is more like a currency and limited usage while NEO is not only used as currency but on its platform ICO projects can deploy their smart contracts like ethereum , however in compare to ether it is not that good but potential to be competitor of ethereum in future .
so NEO will be a good choice to buy and also now it is priced at 30 USD which is really best deal . also to balance your portfolio buy some litecoins also .