Avoidance of dairy products due to lactose intolerance can lead to insufficiency of calcium (Ca) in the body. In an approach to address this problem, tuna bone powder (TBP) was formulated as a calcium supplement to fortify bakery products. In a study, TBP recovered by alkaline treatment contained 38.16 g/100 g of calcium and 23.31 g/100 g of phosphorus. The ratio of Ca:P that was close to 2:1 was hence comparable to that in human bones. The availability of calcium in TBP was 53.93%, which was significantly higher than most calcium salts, tricalcium phosphate (TCP) being the exception. In vitro availability of calcium in TBP-fortified cookies or TCP-fortified cookies were comparable at 38.9% and 39.5%, respectively. These values were higher than the readings from TBP-fortified bread (36.7%) or TCP-fortified bread (37.4%). Sensory evaluation of bakery products containing TBP or TCP elicited comparable scores for the two additives from test panels. Hence, TBP could be used in the production of high calcium bakery products that would enjoy consumer acceptance.