The Acadian and Neoacadian orogenies are widely recognized, yet poorly understood, tectono-thermal events in the New England Appalachian Mountains (USA). We quantified two phases of Paleozoic crustal thickening using geochemical proxies. Acadian (425–400 Ma) crustal thickening to 40 km progressed from southeast to northwest. Neoacadian (400–380 Ma) crustal thickening was widely distributed and varied by 30 km (40–70 km) from north to south. Doubly thickened crust and paleoelevations of 5 km or more support the presence of an orogenic plateau at ca. 380–330 Ma in southern New England. Neoacadian crustal thicknesses show a strong correlation with metamorphic isograds, where higher metamorphic grade corresponds to greater paleo-crustal thickness. We suggest that the present metamorphic field gradient was exposed through erosion and orogenic collapse influenced by thermal, isostatic, and gravitational properties related to Neoacadian crustal thickness. Geobarometry in southern New England underestimates crustal thickness and exhumation, suggesting the crust was thinned by tectonic as well as erosional processes.