Abstract Background Cities contribute more than 70% of global anthropogenic carbon dioxide (CO2) emissions and are leading the effort to reduce greenhouse gas (GHG) emissions through sustainable planning and development. However, urban greenhouse gas mitigation often relies on self-reported emissions estimates that may be incomplete and unverifiable via atmospheric monitoring of GHGs. We present the Hestia Scope 1 fossil fuel CO2 (FFCO2) emissions for the city of Baltimore, Maryland—a gridded annual and hourly emissions data product for 2010 through 2015 (Hestia-Baltimore v1.6). We also compare the Hestia-Baltimore emissions to overlapping Scope 1 FFCO2 emissions in Baltimore’s self-reported inventory for 2014. Results The Hestia-Baltimore emissions in 2014 totaled 1487.3 kt C (95% confidence interval of 1158.9–1944.9 kt C), with the largest emissions coming from onroad (34.2% of total city emissions), commercial (19.9%), residential (19.0%), and industrial (11.8%) sectors. Scope 1 electricity production and marine shipping were each generally less than 10% of the city’s total emissions. Baltimore’s self-reported Scope 1 FFCO2 emissions included onroad, natural gas consumption in buildings, and some electricity generating facilities within city limits. The self-reported Scope 1 FFCO2 total of 1182.6 kt C was similar to the sum of matching emission sectors and fuels in Hestia-Baltimore v1.6. However, 20.5% of Hestia-Baltimore’s emissions were in sectors and fuels that were not included in the self-reported inventory. Petroleum use in buildings were omitted and all Scope 1 emissions from industrial point sources, marine shipping, nonroad vehicles, rail, and aircraft were categorically excluded. Conclusions The omission of petroleum combustion in buildings and categorical exclusions of several sectors resulted in an underestimate of total Scope 1 FFCO2 emissions in Baltimore’s self-reported inventory. Accurate Scope 1 FFCO2 emissions, along with Scope 2 and 3 emissions, are needed to inform effective urban policymaking for system-wide GHG mitigation. We emphasize the need for comprehensive Scope 1 emissions estimates for emissions verification and measuring progress towards Scope 1 GHG mitigation goals using atmospheric monitoring.