According to one aspect, implantable or insertable medical devices are provided, which contain polymeric release regions that release one or more therapeutic agents. The polymeric release regions, in turn, contain the following: (i) a first bonding polymer having a first polymer block and a first bonding group and (ii) a second bonding polymer having a second polymer block and a second bonding group. A therapeutic agent is disposed beneath or within the polymeric release region. The first and second polymer blocks can be the same as or different from one another, as can the first and second bonding groups. The first and second bonding groups are bound to one another via non-covalent bonding, for example, via electrostatic interaction, coordinative bonds, π-π stacking, or hydrogen bonding. According to another aspect, implantable or insertable medical devices are provided, which have a polymeric region that comprises (a) a first polymer having a first polymer block and a first bonding group and (b) a therapeutic agent having a bonding group that bonds to said first bonding group via non-covalent bonding at ambient temperature.