In this work, photosensitive alginate and cellulose-based hydrogels with interpenetrating polymer networks were successfully prepared from alginate, TEMPO-oxidized cellulose nanofibers (TEMPO-CNFs) and polyacrylamide, crosslinked by both Fe3+ and N,N′-methylenebis-acrylamide. The obtained hydrogels showed a clear relationship between the mechanical properties and the content of the TEMPO-CNFs. The results indicated that the mechanical properties of crosslinked hydrogels were enhanced with the mass ratio of TEMPO-CNFs and alginate increased from 1/2 to 2. Moreover, the crosslinked ionic alginate and cellulose-based hydrogels with various TEMPO-CNFs contents exhibited an interconnected porous morphology with an average pore size of ca. 130 µm, and demonstrated an increased cumulative release amount of BSA drugs under the ultraviolet irradiation. This study demonstrated that the as-prepared photoresponsive hydrogels would have a potential application as local drug release systems for wound dressings.