This paper presents new experimental measurements of the laminar flame velocity of components of natural gas, methane, ethane, propane, and n-butane as well as of binary and tertiary mixtures of these compounds proposed as surrogates for natural gas. These measurements have been performed by the heat flux method using a newly built flat flame adiabatic burner at atmospheric pressure. The composition of the investigated air/hydrocarbon mixtures covers a wide range of equivalence ratios, from 0.6 to 2.1, for which it is possible to sufficiently stabilize the flame. Other measurements involving the enrichment of methane by hydrogen (up to 68%) and the enrichment of air by oxygen (oxycombustion techniques) were also performed. Both empirical correlations and a detailed chemical mechanism have been proposed, the predictions being satisfactorily compared with the newly obtained experimental data under a wide range of conditions.