Heart diseases are one of the main causes of mortality worldwide. Various therapies, including cell-, drug-, and biomaterial-based approaches, aim to restore cardiac function. However, their efficacy remains modest, largely due to low retention in the pulsating and dense and cardiac tissue. Injectable hydrogels show promise in cardiac regeneration, offering improved drug delivery, stability, and retention at the target site with minimally invasive administration. In this thesis, the supramolecular ureido-pyrimidinone (UPy) hydrogel is explored, which exhibits pH and temperature responsiveness, facilitating injection and gelation at physiological conditions. On a fundamental level, the modularity and adaptability of UPy-based hydrogels is shown. Different types of UPy-based hydrogel show high cellular-compatibility, and introduction of guest-molecules, which mimic drug moieties, exhibit different mobility and display a sustained release profile. On an application level, a novel in vivo tracking method tested in porcine hearts is developed. Overall, this thesis provides insights into UPy-based hydrogels, functionalization strategies, versatility, and biological applicability, emphasizing their role as a promising delivery platform in cardiac regeneration.

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