Concrete slurry waste (CSW) has the potential of capturing or sequestering CO2. This study designed the low-carbon artificial lightweight cold-bonded aggregates with ultra-high volume of CSW, OSP and MSWIBA (CSW-ALCBAs), and the CO2 sequestrating, compressive strength, and physical properties, leaching toxicity and CO2 emissions of CSW-ALCBAs were investigated. Meanwhile, a novel carbonization device was designed to quantitatively evaluate the potential of CSW-ALCBAs for CO2 adsorption. The results show that both OSP and MSWIBA have the effect of enhancing the CO2 sequestration of CSW-ALCBAs. Besides, the strength, water absorption and apparent density of CSW-ALCBAs also satisfy the demands of GB/T 17461.1–2010. CSW-ALCBAs also exhibit excellent ability to solidify heavy metals and the removal rate of heavy metals is above 80% excepting Cr. ALCBAs with 85% CSW+5% OSP+10% MSWIBA can absorb 29.1313 kg of CO2 (1000 kg ALCBAs), has the highest compressive strength of 1.3 MPa after curing 28 days, water absorption rate is 15.05% and apparent density is 1.3318 g/m3. Overall, this innovative design of CSW-augmented ALCBAs can open up a new area of CSW application that develops technically feasible and cost-efficient carbon-negative building materials.