Semiconductor nanoparticle based porous 3D assemblies are interesting materials for various applications in the fields of photovoltaics, catalysis, or optical sensing. For use as photoelectrodes in photoelectrochemical sensors they need to be characterised by a high porosity, a good photostability, and a high charge carrier mobility. Our work reports on the preparation of cryoaerogel photoelectrodes based on CdSe nanoplatelets and their photoelectrochemical characterisation by means of linear sweep voltammetry (LSV) and intensity modulated photocurrent spectroscopy (IMPS). The obtained open-pored cryoaerogel films were observed to produce much higher photocurrents than comparable drop-cast films. By means of IMPS, the performance differences could be linked to the occurrence of charge carrier movement, which could solely be proven for the cryoaerogels. In a proof-of-principle experiment, the potential of the prepared photoelectrodes for application in photoelectrochemical sensing was moreover demonstrated.