Barite concrete composite materials have been investigated for 252Cf spontaneous neutron and 60Co/192Ir gamma sources’ shielding using Monte Carlo computational method. The Particle and Heavy Ion Transport code System (PHITS) was used to compute the shielding properties of three different materials (barite concrete, barite cement, and barite aggregate) used as structural walls in fixed neutron & gamma industrial radiography for Non-Destructive Testing applications. The obtained results displayed good properties of barite concrete in shielding spontaneous neutrons emitted from the 252Cf source, as the effective dose drops about 108 times in only 140 cm wall thickness, and it was found to be about 10 times more effective than other materials investigated. In addition, the investigated gamma shielding properties of the barite concrete showed a relatively smaller wall thickness compared to the ordinary concrete. The decision-making process based on the ALARA principle of dose limitation showed that the use of barite concrete in such facilities is more effective than the use of barite cement and barite aggregate, for both gamma and neutron radiography shielding design. To achieve an average value of 1 μSv/h, the obtained result shows that 80 cm of Barite concrete is needed, while 125 and 130 cm of barite cement and barite aggregate are needed, respectively to shield the Co-60 source. Meanwhile, 50 cm of wall made of barite concrete is sufficient to cut down the effective dose rate to 1 μSv/h (for 50 Ci and 55 cm for 150 Ci 192Ir), which is an appropriate design for the public area adjacent to the industrial radiographic facility. It was therefore concluded from the obtained data that barite concrete is the most effective shielding material for radioactive sources (60Co, 192Ir, and 252Cf) used in radiographic applications.