This study investigates the effectiveness of alkaline and cementitious additives in the in situ stabilization of localized acid-generating tailings from a closed gold mine in Abitibi–Témiscamingue, Québec (Eagle/Telbel mine site). Five field cells (including one control) were constructed and equipped with mechanisms for collecting vertical water infiltration and surface runoff. The five cells included: (C1) Control cell; (C2) 5 wt % limestone amendment; (C3) 10 wt % limestone amendment; (C4) 5 wt % half ordinary Portland cement and half fly ash amendment; and (C5) 5 wt % ordinary Portland cement amendment. The control cell showed an acidic behavior (pH < 4.5) with variable concentrations of Fe, Al, Zn, and Cu. The amendments were used to neutralize the acidic leachates and decrease dissolved metal concentrations. Leachates from surface runoff samples of amended cells were less loaded with metals compared to samples of vertical infiltration. All amendment formulations increased the pH of the leachates from approximately 4 to circumneutral values. Furthermore, metal and metalloid concentrations were greatly limited, except for Cr and As for the carbonate-based amendments. Metal(-oid) stabilization was successfully achieved using the different amendment formulations, with the exception of C2, which still released As.