"I learn Chinese using a computer."
Communicatively I think it is but you would be changing the grammar making 'use' 用 the main clause verb. The problem grammatically is that in both languages your main clause verb is with the 学习 and the 用 is part of the adj clause present participle (ie ...ing clause). In Chinese these clause phrases are 'fronted' rather than 'reared'. It's just like a prep clause like "at my home'" (zai jia) can't be put at the end as you can in English