Absolutely! It would make it go really rather well with the extra torque! The gearboxes on Smart cars aren't too bad, other than taking an age to change (electric auto changes), but as it would drive in just the one gear I don't expect that would be such a problem. The main problem would be space for battery packs - there's a small amount in the boot and more space under the bonnet.
What battery packs are you using for your conversion?