Molecular dynamics simulations were used to investigate the vapor-liquid equilibria (VLE) and interfacial properties of binary mixtures of N2 with either ethane, propane, n-decane, or n-dodecane. Alkanes and N2 were modeled by using the TraPPE-UA and Rivera force fields, respectively. The typically used Lorentz-Berthelot combining rules resulted in liquid phases that are too N2-rich compared to experiment. To improve the accuracy of VLE predictions, the hydrocarbon-nitrogen interactions were fine-tuned, and these improved parameters were used to investigate interfacial properties. Scaling the interaction strength between nitrogen and -CH3 and -CH2- groups by factors of 0.95 and 0.85, respectively, relative to the Lorentz-Berthelot value, was found to minimize error in pressure-composition phase diagrams. These scaling parameters gave excellent agreement with experimental phase diagrams for mixtures of N2 with ethane, propane, or n-dodecane over a range of state points. For ethane/N2 and n-decane/N2 mixtures, trends in surface tension as a function of temperature and pressure are correctly reproduced, although the simulated values are slightly too high compared to experimental values. To assess how the accuracy of hydrocarbon-N2 interaction strength impacts interfacial property predictions, we have compared density profiles and surface tension using several different scaling factors. Using the Lorentz-Berthelot combining rules rather than optimized parameters gave the same qualitative trends, although some quantitative results, such as liquid-phase N2 mole fraction, were found to differ by a factor of ∼1.5. Using the optimized interaction parameters, interfacial behavior was examined by calculating density and free energy profiles. Nitrogen molecules preferentially adsorb at the interfacial region between the liquid and vapor phases. This interfacial adsorption becomes less energetically favorable as either the temperature, pressure, or length of the alkane chain increases.