Heavy metal pollution in soil can have detrimental effects on soil ecosystems and human health. In situ remediation techniques are widely used to reduce the bioavailable fractions of heavy metals in soil. The main objective of this study was to examine the reduction of the bioavailable fractions of As and Pb in paddy soil with artificial lightweight material (ALM) manufactured from recycled materials. A total of four treatments, including a control (no amendment), ALM10 (10% of ALM in soil), ALM10+L (10% ALM combined with 0.5% lime), and ALM10+FeO (10% ALM combined with 0.5% FeO), were applied to paddy fields, and rice (Oryza sativa L.) was cultivated after 32 weeks. The highest reduction efficiencies for the bioavailable fractions of As and Pb in soil were observed in the ALM10+FeO (52.8%) and ALM10+L treatments (65.7%), respectively. The uptake of As decreased by 52.1% when ALM10+FeO was applied to paddy soil, and that of Pb decreased by 79.7% when ALM10+L was applied. Correlation analysis between bioavailable heavy metals in soil and soil chemical properties showed that soil pH, electrical conductivity (EC), P2O5, and soil organic matter (SOM) were the main factors controlling the mobility and bioavailability of As and Pb. Overall, the efficiencies of As and Pb reduction increased synergistically in both soil and plants when FeO and lime were combined with the ALM. In future studies, long-term monitoring is necessary to examine the longevity of soil amendments.