Seismic anisotropy beneath eastern North America, as expressed in shear wave splitting observations, has been attributed to plate motion‐parallel shear in the asthenosphere, resulting in fast axes aligned with the plate motion. However, deviations of fast axes from plate motion directions are observed near major tectonic boundaries of the Appalachians, indicating contributions from lithospheric anisotropy associated with past tectonic processes. In this study, we conduct anisotropic receiver function (RF) analysis using data from a dense seismic array traversing the New England Appalachians in Connecticut to examine anisotropic layers in the crust and upper mantle and correlate them with past tectonic processes as well as present‐day mantle flow. We use the harmonic decomposition method to separate directionally‐dependent variations of RFs and focus on features with the same harmonic signals observed across multiple stations. Within the crust, there are multiple features that may be correlated with stratification in the Hartford Basin, faults in the Taconic thrust belt, shear zones formed during Salinic/Acadian terrane accretion events, and orogen‐parallel crustal flow in the Acadian orogenic plateau. We apply a Bayesian inversion method to obtain quantitative constraints on the direction and strength of intra‐crustal anisotropy beneath the Hartford Basin. In the upper mantle, we identify a fossil shear zone possibly formed during oblique subduction of Rheic Ocean lithosphere. We also find evidence for a plate motion‐parallel flow zone in the asthenosphere that is likely disturbed by mantle upwelling near the southern margin of the Northern Appalachian Anomaly in the eastern part of the study area.