Background/Objectives: Modern dentistry increasingly requires biomaterials that not only replace damaged tissues but also actively regulate healing processes, modulate inflammation, and provide controlled delivery of therapeutic agents under the complex physicochemical conditions of the oral cavity. This review aims to analyze the potential of PCHs, particularly methacryloyl gelatin (GelMA), as multifunctional platforms for drug delivery in dental applications. Methods: This review provides a structured narrative synthesis of the literature, focusing on the physicochemical, biological, and translational aspects of photocrosslinkable hydrogels in dentistry. Special attention was given to the key functional requirements for hydrogels used in dentistry, including adhesion in a wet environment, antimicrobial properties, and the ability to provide sustained and localized release of active compounds. Natural, synthetic, and semi-synthetic polymers were comparatively evaluated to justify the selection of GelMA as a leading platform due to its tunable mechanical properties, biocompatibility, and photopolymerization capacity. The review also analyzes mechanisms of drug release activation and provides a comparative assessment of commonly used photoinitiators, including Irgacure 2959, lithium phenyl-2,4,6-trimethylbenzoylphosphinate (LAP), and camphorquinone, with emphasis on their cytocompatibility with oral tissues. Results: Applications of these hydrogels in endodontics, periodontology, peri-implantitis therapy, and regeneration of bone and dental pulp are summarized. Conclusions: Overall, photocrosslinkable GelMA-based hydrogels (PC-GelMA) represent promising multifunctional platforms for localized drug delivery and regenerative strategies in modern dentistry.