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Understanding the interactions between the single components of hybrid systems is essential to drive the development of advanced functional materials. A prerequisite for this is the systematic variation of the building blocks of such compounds. Focusing on spiropyran@metal-organic framework (MOF) composite materials with noncovalently attached spiropyran dyes, both the host scaffold and the dye molecules can be systematically tuned. In this work, a broad substitution pattern was applied to systematically elucidate the characteristics of the resulting hybrid materials as a function of the supplemental substitution on spiropyran. The newly developed 12 composites exhibit substitution and host-dependent optical characteristics, which are particularly affected by the substitution of the 6'-position on the chromene ring. Through the favorable combination of the MOF host's polarity and an adequate strength of the spiropyran's indolinedonor-chromeneacceptor pair, reversible conversion between photoisomers is efficiently accomplished, especially for nitro-substituted spiropyrans inside MIL-68(In).