The mechanical removal of dentinal caries traditionally involves the use of tactile sensation and/or caries-indicating dyes. This study tested the hypothesis that self-limiting polymer burs are as effective as conventional carbide burs in creating substrates for dentin bonding. Carious dentin from extracted human molars was removed with carbide or polymer burs, with dental explorer hardness as the end-point for caries removal. Dentin substrates were bonded with etch-and-rinse or self-etch adhesives and prepared for microtensile bond testing and transmission electron microscopy. For each bur type, there was no difference in bond strength between adhesives. However, the polymer bur surface exhibited significantly lower bond strengths than the carbide bur, and both were lower than flat, non-carious dentin controls. TEM revealed areas of incompletely removed, denatured caries-infected dentin in the polymer bur specimens. These first-generation polymer burs might best be utilized for deep caries removal where pulpal exposure is a concern.