The present invention discloses a method for aluminum-enhanced dealkalization of red mud and separation and recovery of aluminum and iron. The method includes: dissolving red mud in water, introducing excessive SO2, introducing O2 for aeration, and refluxing part of alkaline leachate after filtering; when pH of a red mud mixture decreases to below 3, washing and filtering the red mud mixture, adding NaOH to acidic leachate to adjust its pH to a strongly alkaline level, aging and filtering the leachate, treating filter residue to recover Fe2O3, and refluxing part of alkaline leachate after filtering to the red mud mixture; and adjusting pH of the remaining alkaline leachate after filtering to a weakly acidic level, and conducting filtering to recover aluminum.