Can easily walk from Inner Harbor to Mt Vernon (15 min); Federal Hill (5-10 min) or Fells Point 10-15 min). All three neighborhoods have a ton of options. Could take the 94 to Hampden, roughly 30 min ride; just be aware it's not very frequent service; Hampden is a quaint walkable neighborhood with tons of options. Upper Fells and Canton as well, lot of options but I feel like nothing that warrants the trip, but if you feel like it it's about 15-20 min ride on either the 65 or the NV from inner harbor (65 is best if you are going to Canton Square)