For the first time, the hazardous chrysotile was valorized as an aggregate in radiation shielding concrete (RSC). This was accomplished through its amalgamation with two different ratios of boric acid (H3BO3) by 1 and 3% of cement mass to produce CR1, and CR2 concrete mixtures, respectively, in comparison with zero H3BO3 in the control concrete (CC). Physico-mechanical, hydration, and microstructural properties of these concrete mixtures were analyzed employing X-ray diffraction (XRD), Fourier transformation infrared spectroscopy (FTIR), X-ray fluorescence (XRF), scanning electron microscopy (SEM), thermogravimetry/its derivative (TG/DTG), and physico-mechanical tests. Additionally, the radiation shielding was evaluated using Pu–Be, and 60Co sources. Computational studies using NXcom, and WinXCom, as theoretical calculation programs accompanied by the MCNP-5 code as a simulation tool, were applied to verify the radiation shielding measurements. The findings showed that the CC has reasonable radiation shielding with acceptable physico-mechanical properties. On the contrary, CR1 and CR2 had deleterious mechanical and microstructural properties, but more enhanced neutron shielding properties compared to their precursor CC. This conclusion was verified by the remarkable compatibility between the computational and experimental outcomes. Ultimately, H3BO3 additions boosted the radiation shielding of chrysotile concrete despite their devastating impact on the mechanical and microstructural properties, emphasizing the eligibility of chrysotile as an aggregate in RSC. © 2023 Elsevier Ltd.