over, they are often invasive, [2] require high vacuum, [3] or preclude real-space information, [4] thus preventing in situ studies of materials. These two characterization levels are also reflected in current research efforts, for instance, on metalorganic frameworks (MOFs) that mainly focus on two distinct aspects: molecular structures being tuned and bulk properties being measured. [5] MOF chemists often vary the molecular building units (e.g., installation of a functional group) and examine the corresponding change in the performance of a bulk sample (e.g., gas adsorption isotherm). Alteration of MOF particle properties can be caused twofold: (1) by differences in "extrinsic properties", that is, physical parameters like their particle size, shape, and surface structure, or (2) by variations in "intrinsic properties" ruled by chemical attributes of the framework. These include casual differences in the composition of building blocks, [6] crystallinity, [7] functionalization, [8] and defects, [2] but also designed variations as in multivariate MOFs. The interplay of both kinds of properties determines the overall performance for any application; the mutual impact of intrinsic and extrinsic variations correlated to any change in individual particle properties in situ is challenging to explore in a correlative manner.At present, an enormous characterization gap exists between the study of the crystal structure of a material and its bulk properties. Individual particles falling within this gap cannot be fully characterized in a correlative manner by current methods. The authors address this problem by exploiting the noninvasive nature of optical microscopy and spectroscopy for the correlative analysis of metal-organic framework particles in situ. They probe the intrinsic as well as extrinsic properties in a correlated manner. The authors show that the crystal shape of MIL-88A strongly impacts its optical absorption. Furthermore, the question of how homogeneously water is distributed and adsorbed within one of the most promising materials for harvesting water from humid air, MOF-801, is addressed. The results demonstrate the considerable importance of the particle level and how it can affect the property of the material.