As part of a comprehensive study on eco-friendly processing techniques, the influence of the heat treatment environment on the case hardening of AISI 1018 steel using pulverized cassava leaf was studied. The process was carried out at two different temperatures (850 °C and 950 °C) and under three environmental conditions: Process 1, the control experiment, was carried out in air only; in Process 2, the medium comprised pulverized cassava leaves; and in Process 3 a combination of pulverized cassava leaves plus barium carbonate (BaCO3) was used as an energizer (CBC mixture). Vickers microhardness testing and scanning electron microscopy were used to evaluate the effect of the processing environment on the case hardening of the steel. As expected, regardless of the processing temperature, Process 1 resulted in little or no hardening of the steel surface. However, notable case hardening occurred when the steel specimens were subjected to either Process 2 or Process 3. Furthermore, the inclusion of barium carbonate in Process 3 significantly enhanced the case hardening effectiveness of the cassava leaf in terms of the rate of and maximum hardness achieved. A maximum enhancement was observed at 950 °C. After 1 h, the increase in hardness was 160% and 280% for Process 2 and Process 3, respectively. Upon increasing the processing time to 5 h, the increase in hardness due to Process 2 was raised to 254%, while that of Process 3 remained at approximately 280%. The diffusivity of AISI 1018 was calculated using the microhardness data. The diffusivity was highest in Process 2 samples with values of 1.568 × 10−9 m2/s at 850 °C and 1.893 × 10−9 m2/s at 950 °C. Effective case hardening of AISI 1018 steel was carried out using the medium of cassava leaf, without the addition of barium carbonate (BaCO3) as an energizer.