There is a pressing need for well-informed management to reduce wildfire hazard and restore fire's beneficial ecological role in the Mediterranean- and temperate-climate forests of California, USA. These efforts rely upon the accessibility of high spatial and temporal resolution data on biomass and canopy fuel parameters such as canopy base height (CBH), mean canopy height, canopy bulk density (CBD), canopy cover, and leaf area index (LAI). Remote sensing using unoccupied aerial system Structure-from-Motion (UAS-SfM) presents a promising technology for this application due to its accessibility, relatively low cost, and possibility for high temporal cadence. However, to date, this method has not been studied in the complex mosaic of forest types found across California. In this study we examined the capacity of structural and multispectral information obtained from UAS-SfM, in conjunction with machine learning methods, to model aboveground biomass and forest canopy fuel structural parameters using an area-based approach across multiple sites representing a diversity of forest types in California. Based on correlations with field measurements, fuel parameters separated into vertical (biomass, CBH, and mean height) and horizontal (LAI, CBD, canopy cover) groups. UAS-SfM random forest models performed well for modelling the vertical structure canopy fuels parameters (R2 0.69–0.75). These models exhibited strong performance in comparison to ALS, as well as when transferred to a novel site. Vertical structure predictors were prominent in these models, and did not improve with the addition of spectral predictors. UAS-SfM random forest models of horizontal structure parameters mainly used raster-based spectral indices (primarily NDVI) and had relatively low performance (R2 0.49–0.59). In addition, these models underperformed ALS and had poor performance when applied to a novel site. When applied to a region with widespread UAS-SfM coverage, models from both groups successfully produced contiguous maps that could be used for modelling fire behavior or in management decision making and monitoring. These findings indicate that UAS-SfM, without the need for multispectral sensors, is well suited for mapping area-based vertical-structure canopy parameters across diverse landscapes supporting a wide range of forest types. In contrast, the identification of spectral mean variables for modelling horizontal structure canopy fuels suggests the potential of multi- or hyperspectral sensors or high-resolution satellite imagery for meeting management information needs.