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Assessing the K isotopic composition of the upper continental crust is important for understanding the processes by which the crust is generated and modified, and constraining the K isotopic budget of the silicate Earth. High-precision K isotopic data are reported for 70 well-characterized individual and composite samples from the upper continental crust, including diorite, granodiorite, granite, loess, shale, graywacke, pelite, and tillite, to constrain its K isotopic composition. δ41K varies significantly in eight I-type and two S-type granites from Australia (−0.57 to −0.40‰), nine A-type granites (−0.53 to −0.38‰), and three granitoid composites including diorite, granodiorite, and granite (−0.50 to −0.37‰) from China, mainly reflecting source heterogeneity. The 22 post-Archean Australian shales (PAAS) (δ41K = −0.68 to −0.12‰) and the 12 sedimentary composites including graywacke, pelite, and tillite from China (δ41K = −0.57 to −0.23‰) have heterogeneous K isotopic compositions while the 12 loess samples from around the world display more limited K isotopic variation (δ41K = −0.47 to −0.35‰). δ41K values display a smaller dispersion in loess compared to shales, which have comparatively more intense weathering and higher chemical index of alteration (CIA). δ41K correlates with Fe 2 O 3 /Al 2 O 3 and Fe 2 O 3 /K 2 O in shales and Al 2 O 3 /SiO 2 , K 2 O/Al 2 O 3 , and δ7Li in loess, suggesting that K isotopes are fractionated during chemical weathering. Overall, the upper continental crust has a heterogeneous K isotopic composition, ranging from −0.68 to −0.12‰ with an average δ41K of −0.44 ± 0.05‰ (2SD, n = 88), which is indistinguishable from the mantle. [ABSTRACT FROM AUTHOR]