This paper focuses on the combustion chemistry of 2-methylfuran (2-MF), a potential biofuel, and it is built on the previous work of Tran et al. [Combust. Flame 161 (2014) 766]. In their work, they had combined detailed flame chemistry modeling with flame speciation data based on flame-sampling molecular beam mass spectrometry (MBMS) with electron ionization and gas chromatography with MS detection. In this work, we significantly extend those previous studies by in-situ isomer-resolving species identification and quantification. Specifically, we have determined the detailed chemical structure of a premixed laminar 2-MF flame using flame-sampling high-resolution MBMS with synchrotron-generated vacuum-ultraviolet radiation. Mole fraction profiles of 60 intermediate, reactant, and product species were measured in order to assess the pollutant potential of this possible next-generation biofuel. Special emphasis is paid towards the fuel's ability to form aromatic and oxygenated intermediates during incomplete combustion processes, with the latter species representing a variety of different classes including alcohols, ethers, enols, ketones, aldehydes, acids, and ketenes. Whenever possible the experimental data are compared to the results of model calculations using the 2-MF combustion chemistry model of Tran et al. , but it should be noted that many newly detected species are not included in the calculations. The experimental data presented in this work provides guidance towards to development of a next-generation 2-MF combustion chemistry model.