The controls on potassium (K) isotope fractionation during chemical weathering are evaluated using two regolith profiles developed over ∼350 kyr on the humid and arid sides of Kohala Mountain, Hawai‘i. The humid regolith shows 145% K enrichment relative to the basaltic parent in shallow (≤1 m) horizons, but losses of up to 90% in the deeper horizons. By contrast, the arid regolith has lost between 60 and 90% K from the top 1 m of the soil with the least depletion in the deeper horizons due to limited chemical weathering. This apparent contradiction can be explained by enhanced accumulation of K-bearing mineral aerosols in the humid regolith. Bulk δ41K varies from −0.76 ± 0.08 to −0.31 ± 0.06‰ in the humid regolith compared with −0.48‰ for the underlying basalt. In contrast, the arid regolith shows δ41K values ranging from −0.39 ± 0.10 to −0.02 ± 0.05‰, heavier than that of their basaltic parent. Exchangeable (NH4Ac extracts) δ41K of the humid and arid regoliths ranges from −0.63 ± 0.07 to 0.11 ± 0.07‰ and −0.01 ± 0.05 to 0.04 ± 0.08‰, respectively. Exchangeable K has δ41K higher than (or similar to) the bulk values in most samples, reflecting a potential contribution of marine aerosols to the labile (plant available) K pool. In the shallow regolith, K derived from mineral aerosols is significant, especially for the humid site, and this idea is supported by enriched quartz, radiogenic Nd-Sr isotope values towards the surface, and increasing δ41K close to the upper crustal composition (an analogue of the dust). The enrichment of K in humid surface soils, an upward decrease in exchangeable δ41K in the humid regolith and plant-like δ41K in the topmost, organic-rich soils may reveal the contribution of plant cycling. Low δ41K in deep, humid regolith relative to δ41KBasalt appears to be driven by clay incorporation of isotopically light K. In comparison, higher δ41K in the arid regolith than δ41KBasalt likely reflects an interplay between preferential clay 41K sorption in alkaline environments and preservation of seawater-derived K in forms of clay adsorbed complex and carbonate phases (via adsorption and/or incorporation). Our results reveal that the K isotope composition in Hawaiian regoliths depends on climate, while it is complicated by the interaction among weathering, plant cycling and addition of marine and mineral aerosols.