Mixed-matrix membranes (MMMs) formed by incorporating metal-organic frameworks (MOFs) into polymers have ag eneral limitation in that the MOFs are typically formed into rather simple dimensionalities (such as 1D, 2D, or 3D). Each design approachh as intrinsic-albeit independent-benefits, such as network percolation (1D), access to high-aspect ratios (2D), and ease of processability (3D). However, ad esign strategyi s neededt oc ombine multiple dimensionalitiesa nd, thereby, access the full range of transport and compositingb enefits of these high-performance materials. Herein, af acile method to form multi-dimensional HKUST-1n anoparticles is introduced by using am odulator to tune the MOF nucleation and growth mechanism. At 30 wt %m ultidimensional MOF loading, the MMM shows CO 2 permeabilities of approximately 2500 Barrer, which represents a2 .5-fold increase compared to that of a pure polymer without al arge loss of selectivity for CO 2 /CH 4 and CO 2 /N 2 .A dditionally,a lmost no plasticization pressure response is observed for CO 2 up to 750 psi, suggesting an unusual stability to high activity feeds.[a] W.Supporting Information and the ORCID identification number(s) for the author(s) of this article can be found under: https://doi.