Electron spins in molecular systems provide a promising platform for quantum technologies due to their chemical tunability and potential for room-temperature operation. These spin states can be optically initialized and manipulated, while the transfer of spin information back to light enables spin-photon interfaces. However, achieving efficient optical readout and control of molecular electron spins under ambient conditions remains challenging. In this talk, Dr Grüne will present approaches based on optically detected magnetic resonance (ODMR), electron paramagnetic resonance (EPR), and optical spectroscopy to probe and manipulate spin states, including recent work demonstrating optical readout of high-spin states at room temperature. Dr Grüne will discuss the development of zero-field ODMR, which enables optical spin readout without large magnetic fields or cryogenics, and outline a pathway towards spin-photon interfaces for quantum technologies based on molecular systems.