The construction of molecular crystal materials with physical properties that can be dynamically controllable through various stimuli such as light and electricity is of extraordinary significance, while this remains a tremendous challenge. In this context, we demonstrate two novel 2-D multi-function viologen complexes, {[Ln(bcbp)(BDC)(CH3OH)(H2O)2]·Cl·CH3OH·H2O}n (1-Eu, and 2-Dy; H2bcbp·2Cl = 1,1′-bis(4-carboxyphenyl)-(4,4′-bipyridinium) dichloride; BDC = p-phthalic acid, and Ln = Eu, Dy). Due to the strong π-π interaction between viologen and BDC in the interlocked structure, both compounds exhibit rapid and reversible responses under the stimuli of UV light and electricity. Furthermore, accompanying the photochromic process, photo-modulated luminescent and photomagnetic behavior have been observed. Considering the excellent photochromic performance, the function filter paper and smart organic glass were successfully prepared and used for ink-free printing and UV light filtering.