There is an urgent need for efficient solution-processable p-type semiconductors. Copper(I) iodide (CuI) has attracted attention as a potential candidate due to its good electrical properties and ease of preparation. However, its carrier dynamics still need to be better understood. Carrier dynamics after bandgap excitation yielded a convoluted signal of free carriers (positive signal) and a negative feature, which was also present when the material was excited with sub-bandgap excitation energies. This previously unseen feature was found to be dependent on measurement temperature and attributed to negative photoconductivity. The unexpected signal relates to the formation of polarons or strongly bound excitons. The possibility of coupling CuI to plasmonic sensitizers is also tested, yielding positive results. The outcomes mentioned above could have profound implications regarding the applicability of CuI in photocatalytic and photovoltaic systems and could also open a whole new range of possible applications.