Cadmium presence in soil is considered a significant threat to human health. Biochar is recognized as an effective method to immobilize Cd ions in different soils. However, obtaining effective and viable biochar to remove elevated Cd from postmining soil remains a challenge. More modifiers need to be explored to improve biochar remediation capacity. In this investigation, pot experiments were conducted to study the effects of poplar-bark biochar (PBC600) and thiourea-modified poplar-bark biochar (TPBC600) on Cd speciation and availability, as well as on soil properties. Our results showed that the addition of biochar had a significant influence on soil properties. In the presence of TPBC600, the acid-soluble and reducible Cd fractions were transformed into oxidizable and residual Cd fractions. This process effectively reduced Cd bioavailability in the soil system. Compared to PBC600, TPBC600 was more effective in improving soil pH, electrical conductivity (EC), organic matter (SOM), total nitrogen (TN), ammonium nitrogen (NH4+-N), nitrate nitrogen (NO3--N), available potassium (AK), available phosphorus (AP), and available sulfur (AS). However, this improvement diminished as incubation time increased. Results of Pearson correlation analysis, multivariate linear regression analysis, and principal component analysis showed that soil pH and available phosphorus played key roles in reducing the available cadmium in soil. Therefore, TPBC600 was shown to be an effective modifier that could be used in the remediation of soil polluted with Cd.