Hybrid framework materials are modular compounds consisting of metal ions and organic linkers, variation of which has given rise to a myriad of structures with technologically relevant properties. To date, extensive experimental and theoretical studies have been carried out to understand key factors that affect processes such as gas adsorption, gas separation and heterogeneous catalysis in nanoporous metal-organic frameworks (MOFs).[1] Dense hybrid frameworks are also of growing interest on account of their unique physical properties, such as multiferroics, electronic conductivity and photoluminescence, among others.[2] For all viable applications, the robustness of the materials and, in particular, a detailed understanding of their mechanical properties, are necessary for successful utilization. This field, however, remains largely unexplored. Recent experimental studies [3] have demonstrated that the elastic properties, especially the bulk modulus (B) [4] and the Young's modulus (E) [5] of nanoporous and dense hybrid frameworks, can be correlated to their density, dimensionality and their underlying chemical structures. In addition, recent computational studies have reported that the bulk moduli of a family of isoreticular metal-organic frameworks (IRMOFs) depend on the size of the aromatic organic linkers (which determines the density).[6] Herein, we employed a combination of computational and experimental approaches to probe the elastic properties of a dense and anisotropic hybrid framework material: zinc phosphate phosphonoacetate hydrate, Zn 3 -(PO 4 )(O 2 CCH 2 PO 3 )(H 2 O), 1. [7] We propose an efficient computational scheme for the approximate analysis of the Young's modulus and the Poisson's ratio (n) along the principal directions of an anisotropic crystal. Notably, this approach circumvents the intricacies involved in computing the full elastic stiffness tensor.[8] The validity of our theoretical calculations was confirmed by single-crystal nanoindentation experiments. In addition, theoretical studies were performed by subjecting the anisotropic framework to hydrostatic compression to reveal the role of the basic building blocks.Studies to date indicate that both the local density approximation (LDA) and the general gradient approximation (GGA) levels of density functional theory (DFT) have over-predicted the bulk modulus (B) of MOF materials. By way of an example, the B value of the lightweight MOF-5 (density of 0.59 g cm À3