Lanthanide(III) ion (Ln(III)) sensing has become a major research area owing to its intriguing prospect in clinic, biology, and environmental studies. However, the existing methods have limitations like requirement of expensive instrumentation, long analytical times, and sample pretreatments, revealing the necessity of other methods. In this work, by using N-methyl-4-pyridinium tetrazolate (mptz) zwitterion as an electron acceptor, we obtained several new Ln(III) compounds with electron-transfer (ET) photochromic properties: [Ln(NO3)3(H2O)4]·mptz [Ln = Sm (1), Eu (2), Gd (3), La (4), Ce (5), Pr (6), Nd (7), Tb (8), Dy (9), Ho (10), Er (11), Tm (12), Yb (13), Lu (14)]. Notably, different Ln(III) ions in these compounds can be visually identified by their different photoinduced color changes related to the ET process. This work may not only contribute to the more understanding of the structure-photosensitivity relationships of pyridinium-based compounds, but also provide a new approach for Ln(III) ion sensing.