This body of research uses numerical and experimental investigative techniques to further the understanding of autoignition. Hydrogen/nitrogen and methane/air fuel configurations of turbulent lifted flames in a vitiated coflow burner are used as model flames for this investigation. Characterisation was undertaken to understand the impact of controlling parameters and the overall behaviour of the flames, and to provide a body of data for modelling comparisons. Modelling of the flames was conducted using the PDF-RANS technique with detailed chemistry incorporated using In-situ Adaptive Tabulation (ISAT) within the commercial CFD package, FLUENT 6.2. From these investigations, two numerical indicators for autoignition were developed: convection-reaction balance in the species transport budget at the mean flame base; and the build-up of ignition precursors prior to key ignition species. These indicators were tested in well defined autoignition and premixed flame cases, and subsequently used with the calculated turbulent lifted flames to identify if these are stabilised through autoignition. Based on learnings from the modelling, a quantitative, high-resolution simultaneous imaging experiment was designed to investigate the correlations of an ignition precursor (formaldehyde: CH2O) with a key flame radical (OH) and temperature. Rayleigh scattering was used to measure temperature, while Laser Induced Fluorescence (LIF) was used to measure OH and CH2O concentrations. The high resolution in the Rayleigh imaging permitted the extraction of temperature gradient data, and the product of the OH and CH2O images was shown to be a valid and useful proxy for peak heat release rate in autoigniting and transient flames. The experimental data confirmed the presence of formaldehyde as a precursor for autoignition in methane flames and led to the identification of other indicators. Sequenced images of CH2O, OH and temperature show clearly that formaldehyde exists before OH and peaks when autoignition occurs, as confirmed by images of heat release. The CH2O peaks decrease later while those of OH remain almost unchanged in the reaction zone.