The present investigation describes aluminum-induced changes in the leaves of two buckwheat species using both physiological and biochemical indices. With increasing levels of Al (viz. 100, 200 and 300 μM), the mean length of root, shoot as well as their biomass accumulation decreased linearly with respect to control. Tolerance test of F. kashmirianum revealed that it was more tolerant to Al-stress than F. tataricum as revealed by higher accumulation of Al in its roots without any significant damage. Translocation factor (TF) values of both species were found to be < 1, indicating more Al is restrained in roots. Total chlorophyll showed a non-significant increase in F. tataricum while as decreased in F. kashmirianum at 300 μM concentration besides, the carotenoid content exhibited inclined trend in F. tataricum and showed a concomitant decrease in F. kashmirianum. The anthocyanin level showed a non-significant decline in F. kashmirianum. Exposure to different Al-treatments enhances malondialdehyde (MDA), HO and membrane stability index (MSI) in both species, with increases being greater in F. kashmirianum than F. tataricum as also revealed by DAB-mediated in vivo histo-chemical detection method. The osmolyte level in general were elevated in both buckwheat species however, enhancement was more in F. tataricum than F. kashmirianum. The activities of antioxidant enzymes viz. superoxide dismutase (SOD), ascorbate peroxidase (APX), guaiacol peroxidase (POD), glutathione reductase (GR), glutathione-S-transferase (GST) were positively correlated with Al-treatment except catalase (CAT) which exhibits a reverse outcome in F. kashmirianum. The present investigation could play an essential role to better understand the detoxification mechanisms of Al in plants.