The Environmental Audit Committee report revealed that the coalition's green policies caused an increase in emissions for a number of airborne pollutants in 2013, having been on an even keel between 2010 and 2012, and having been in decline before that.
The negative trend has developed despite the prime minister stating that he wanted to lead "the greenest government ever" in May 2010.
Conservation director at Christian environmental group A Rocha UK, Andy Lester, told Premier's News Hour that David Cameron had serious questions to answer on the issue.
He said: "It is his own party as much as the other parties condemning the government's record on green issues, and so if his own party is saying that then I think can we can be pretty confident of a poor job on most environmental issues."
The report also said that the UK had failed to meet nitrogen dioxide pollution targets in 34 of the 43 zones specified in the EU directive on air quality in 2012, resulting in the European Commission launching infraction proceedings against the UK in February 2014 regarding the 16 zones that would not be compliant by 2015.
In July 2014, the Department for Environment, Food and Rural Affairs (Defra) reassessed the timespan required in order to meet nitrogen dioxide limits, stating that Greater London and two other areas would not meet the required levels until after 2030.
The committee has called for the creation of new legal commitments to protect the environment, claiming that it should be overseen by a new Office for Environmental Responsibility to ensure that all government policies are compatible with those commitments.
The government has said that it strongly disagrees with the findings.
Listen to the full report from Andy Lester at A Rocha UK: