In this study, the effectiveness of powder laser desorption/ionization (LDI) coupled with Fourier-transform ion cyclotron mass spectrometry (FT-ICR MS) was evaluated for the improved coverage of plant metabolites. Ground plant (powder) was fixed on a metal plate using double-sided tape. Compared with the conventional approach involving liquid extraction, which is followed by electrospray ionization MS analysis, a smaller amount of sample (similar to 200 mu g) was required in the proposed method. Additionally, the laborious steps of liquid extraction, concentration, and solid-phase extraction were avoided. Employing the proposed method in Centella asiatica leaves analysis, higher number of reproducible molecular formulas (>5000) and metabolites (>650) were obtained than the conventional methods. Flavonoids, phenolic acids, xanthones, lipids, carbohydrates, terpenoids, and alkaloids compounds were detected from leaves, stems, and roots of C. asiatica. This study indicates that LDI FTICR MS is a quick and effective tool for enhanced plant metabolite profiling in the solid phase.