The Santa Rosa mylonite zone developed predominantly from a granodiorite protolith in the eastern margin of the Peninsular Ranges batholith. A wide variation in K−Ar biotite dates within the zone is shown to reflect the times of cooling through closure temperatures whose variability is chiefly a result of deformation-induced reduction in grain size. We suggest that such variation generally may be exploited to place constraints on the timing of deformation episodes. Previous workers have shown that deformation in the Santa Rosa mylonite zone involved the formation of mylonites and an imbricate series of low-angle faults which divide the area into structural units. Field work, petrographic studies, and TEM analysis of deformation mechanisms in biotite show that the granodiorite mylonite, the lowermost structural unit, formed below the granodiorite solidus. The granodiorite mylonite varies from protomylonite to ultramylonite, with regions of high strain distributed heterogeneously within the zone. Previously reported biotite and hornblende K−Ar dates from the granodiorite protolith below (82–89 Ma) and the Asbestos Mountain granodiorite above (61–68 Ma) the mylonite zone indicate dramatically dissimilar thermal histories for the lowermost and uppermost structural units. Other workers' fission track dates on sphene, zircon, and apatite from the granodiorite mylonite and the Asbestos Mountain granodiorite suggest thermal homogenization and rapid cooling to ∼100° C by ca 60 Ma. Within and adjacent to the mylonite zone, K−Ar dates on 5 samples of biotite from variably deformed granodiorite range from 62–76 Ma; dates are not correlated with structural depth but clearly decrease with degree of deformation and concomitant grain size reduction. 40Ar/39Ar incremental heating analyses of biotite from the granodiorite protolith reveals no evidence of excess argon and produces a relatively flat age spectrum. 40Ar/39Ar incremental heating analysis of biotite from the granodiorite mylonite discloses discordance consistent with 39Ar recoil loss. K analysis of samples, allowing K−Ar dates to be calculated, is therefore recommended as an adjunct to 40Ar/39Ar step heating analysis in rocks that have experienced similar deformation. During mylonitization, biotite grain size reduction through intracrystalline cataclasis results in estimated grain dimensions as small as 0.05 μm locally within porphyroclasts as large as 1 mm. Because biotite compositions are relatively Uniform (Fe/[Fe+Mg+Mn+Ti+AlVI]=0.47–0.52) and show no systematic variation with grain size, compositional dependence of activation energy and diffusivity can be eliminated as sources of variation in Ar retention. Ar closure temperatures, calculated with appropriate diffusion parameters for the observed grain sizes, are in the range ∼220–280° C and define a cooling curve consistent with a thermal history intermediate between those of the granodiorite protolith below and the Asbestos Mountain granodiorite above the mylonite zone. Changes in the slope of the cooling curve indicate that the main deformation episode initiated at or above ca 330° C (∼80 Ma), above the closure temperature for thermally activated diffusion of argon in biotite, and continued to a minimum of ca 220–260° C (∼62 Ma).