Historical gold mining operations between the 1860s and 1940s have left substantial quantities of arsenic- and mercury-rich tailings near abandoned mines in remote and urban areas of Nova Scotia, Canada. Large amounts of materials from the tailings have entered the surface waters of downstream aquatic ecosystems at concentrations that present a risk to benthos. We used paleolimnological approaches to examine long-term trends in sedimentary metal(loid) concentrations, assess potential sediment toxicity, and determine if geochemical recovery has occurred at four lakes located downstream of three productive gold-mining districts. During the historical mining era, sedimentary total arsenic and mercury concentrations and enrichment factors increased substantially at all downstream lakes that received inputs from tailings. Similarly, chromium, lead, and zinc concentrations increased in the sediments after mining activities began and the urbanization that followed. The calculated probable effects of concentration quotients (PEC-Qs) for sediments exceeded the probable biological effects threshold (PEC-Q > 2) during the mining era. Although sedimentary metal(loid) concentrations have decreased for most elements in recent sediments, relatively higher PEC-Q and continued exceedance of Canadian Interim Sediment Quality Guidelines suggest that complete geochemical recovery has not occurred. It is likely that surface runoff from tailing fields, urbanization, and climate-mediated changes are impacting geochemical recovery trajectories.