Time-resolved phosphorescence anisotropy ͑TPA͒ is used to measure the short-time rotational diffusion coefficient D s r () of charged tracer spheres as a function of the volume fraction of like-charged colloidal host spheres in nonaqueous solvents. Sphere interactions are varied from long-range repulsive to short-range attractive by changing the ionic strength and the solvent composition. It is shown that D s r () is very sensitive to details of the interaction near contact, in agreement with theory. In contrast, the low-shear viscosity L () of the host dispersions is mostly controlled by the tail of the interaction potential. We discuss the applicability of Stokes-EinsteinDebye scaling D s r ()ϰ1/ L (), and D s r ()ϰ1/ ϱ (), where ϱ is the high-frequency-limiting viscosity. Scaling with L () fails at high particle and low salt concentrations, while scaling with ϱ is fairly good, in particular when an apparent nonstick boundary condition is imposed on the friction factor. We conclude that TPA is well suited for use as a microrheological technique.