Mitigation of greenhouse gas (GHGs) emissions and improving soil health using biochar (BC) shall help achieving the UN-Sustainable Development Goals. The impacts of walnut shells biochar (WSB) pyrolyzed at different temperatures on CO2 and N2O emission and soil health have not been yet sufficiently explored. We investigated the effects of addition of WSB pyrolyzed at either 300 °C (WSB-300), 450 °C (WSB-450), or at 600 °C (WSB-600) to alkaline soil on CO2 and N2O emissions, nutrients availability, and soil enzymes activities in a 120-day incubation experiment. Cumulative N2O emissions were reduced significantly as compared to the control, by 64.9%, 50.6%, and 36.4% after WSB-600, WSB-450 and WSB-300, respectively. However, the cumulative CO2 emissions increased, over the control, as follows: WSB-600 (50.7%), WSB-450 (68.6%), and WSB-300 (73.4%). Biochar addition, particularly WSB-600 significantly increased soil pH (from 8.1 to 8.34), soil organic C (SOC; from 8.6 to 22.3 g kg−1), available P (from 21.0 to 60.5 mg kg−1), and K (181.0–480.5 mg kg−1), and activities of urease, alkaline phosphatase, and invertase. However, an opposite pattern was observed with NH4+, NO3−, total N and β-glucosidase activity after WSB application. The WBS produced from high temperature pyrolysis can be used for N2O emissions mitigation and improvement of soil pH, SOC, available P and K, and activities of urease, alkaline, phosphatase. However, WBS produced from low temperature pyrolysis can be used to promote N availability and β-glucosidase; however, these findings should be verified under different field and climatic conditions.