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Polyelectrolyte multilayered (PEM) coatings were fabricated to incorporate and release the small, hydrophilic antibiotic gentamicin from implant surfaces for infection control. The use of a cationic hydrolytically cleavable poly(p-amino ester) rendered these films biodegradable, yielding both diffusion-based and surface-erosion based release of this therapeutic. The Layer-by-Layer (LbL) assembly platform was used to create conformal, micron scale reservoirs with highly tunable drug release. Film release profiles were engineered through film architecture design and post-processing crosslinking techniques. Delivery of gentamicin was sustained for weeks, which is a significant improvement from previous gentamicin-releasing LbL systems. To gain better insight on the mechanisms of release and aid in rational film design, a theoretical treatment of the physical system was performed. These results include an analytical mathematical model describing the release of drug per surface area of film as a function of time as well as a computational model that simulates the time-dependent concentration profiles in these LbL systems. These erodible, antibiotic coatings were demonstrated to be bactericidal agains