Considering the in vivo application limits of ultraviolet radiation (i.e., poor tissue penetrability and potential cytotoxicity), the data discussed herein represent the basis for the optimization of a donepezil-like molecule capable of synergistically inhibiting two target enzymes, namely AChE and MAO-B, involved in neurodegenerative diseases, with the added value of the photomodulation of the pharmacological effect, in order to obtain a tool of interest for the personalized medicine of the future. Here, ACHE is linked to neurodegenerative disease.