ABSTRACT We employ a sample of 135 873 RR Lyrae stars (RRLs) with precise photometric-metallicity and distance estimates from the newly calibrated P–ϕ31–R21–[Fe/H] and Gaia G band P–R21–[Fe/H] absolute magnitude–metallicity relations of Li et al., combined with available proper motions from Gaia EDR3, and 6955 systemic radial velocities from Gaia DR3 and other sources, in order to explore the chemistry and kinematics of the halo of the Milky Way (MW). This sample is ideally suited for characterization of the inner- and outer-halo populations of the stellar halo, free from the bias associated with spectroscopically selected probes, and for estimation of their relative contributions as a function of Galactocentric distance. The results of a Gaussian mixture model analysis of these contributions are broadly consistent with other observational studies of the halo, and with expectations from recent MW simulation studies. We apply the hdbscan clustering method to the specific energies and cylindrical actions (E, Jr, Jϕ, Jz), identifying 97 dynamically tagged groups (DTGs) of RRLs, and explore their associations with recognized substructures of the MW. The precise photometric-distance determinations (relative distance errors on the order of 5 per cent or better), and the resulting high-quality determination of dynamical parameters, yield highly statistically significant (low) dispersions of [Fe/H] for the stellar members of the DTGs compared to random draws from the full sample, indicating that they share common star-formation and chemical histories, influenced by their birth environments.