The environmental impact of diesel-fueled buses can potentially be reduced by the adoption of alternative propulsion technologies such as lean-burn compressed natural gas (LB-CNG) or hybrid electric buses (HEB), and emissions control strategies such as a continuously regenerating trap (CRT), exhaust gas recirculation (EGR), or selective catalytic reduction with trap (SCRT). This study assessed the environmental costs and benefits of these bus technologies in Greater London relative to the existing fleet and characterized emissions changes due to alternative technologies. We found a >30% increase in CO2 equivalent (CO2e) emissions for CNG buses, a <5% change for exhaust treatment scenarios, and a 13% (90% confidence interval 3.8-20.9%) reduction for HEB relative to baseline CO2e emissions. A multiscale regional chemistry-transport model quantified the impact of alternative bus technologies on air quality, which was then related to premature mortality risk. We found the largest decrease in population exposure (about 83%) to particulate matter (PM2.5) occurred with LB-CNG buses. Monetized environmental and investment costs relative to the baseline gave estimated net present cost of LB-CNG or HEB conversion to be $187 million ($73 million to $301 million) or $36 million ($-25 million to $102 million), respectively, while EGR or SCRT estimated net present costs were $19 million ($7 million to $32 million) or $15 million ($8 million to $23 million), respectively.