Nitrogen-vacancy (NV) centres in diamond are point-like defects that have attracted a lot of attention as promising candidates for quantum technologies particularly for sensing and imaging nanoscale magnetic fields. For this application, the use of a high NV density within a high-quality diamond layer is of prime interest. In previous works, it has been demonstrated that in situ doping with N2O rather than N2 during chemical vapour deposition (CVD), limits the formation of macroscopic defects and improves NV's photostability. In this work, we focus on the optimization of the CVD growth conditions to obtain a high NV density keeping a constant N2O concentration in the gas phase (100 ppm). For this purpose, freestanding CVD layers are prepared varying two main growth parameters: methane content and substrate temperature. High energy electron irradiation followed by annealing is finally carried out in order to increase the NV yield through partial conversion of N impurities. Defect concentrations and spin properties are investigated. We find that growth under lower methane concentrations and lower temperatures enhances NV doping. NV ensembles with a density of the order of 2 ppm are finally obtained with narrow spin resonance linewidth. In addition, higher annealing temperatures of 1200 °C following irradiation are found to efficiently remove defects thus improving spin properties.