This thesis presents a series of single-shot non-intrusive diagnostics of key attributes of electron bunches produced by a laser-plasma accelerator (LPA). Three injection mechanisms of the LPA are characterized: channeled and self-guided self-injection, plasma down-ramp injection, and two-beam colliding pulse injection. New diagnostic techniques are successfully demonstrated: up to 8 times higher sensitivity wavefront sensor-based plasma density measurements, strong spatiotemporal coupling of the focused THz pulse is demonstrated using the temporal electric-field cross-correlation (TEX) of a long chirped probe with a short probe and confirms the two-component structure of the bunch observed by electron spectrometry, and normalized transverse emittances as low as 0.1 mm mrad are demonstrated for 0.5 GeV-class beams produced in a capillary-guided LPA by characterizing the betatron radiation emitted by the electrons inside the plasma using a new single-shot X-ray spectroscopy technique.