Desktop laser plasma acceleration has proven to be able to generate gigaelectronvolt-level quasi-monoenergetic electron beams. Moreover, such electron beams can oscillate transversely (wiggling motion) in the laser-produced plasma bubble/channel and emit collimated ultrashort X-ray flashes known as betatron radiation with photon energy ranging from kiloelectronvolts to megaelectronvolts. This implies that usually one cannot obtain bright betatron X-rays and high-quality electron beams with low emittance and small energy spread simultaneously in the same accelerating wave bucket. Here, we report the first (to our knowledge) experimental observation of two distinct electron bunches in a single laser shot, one featured with quasi-monoenergetic spectrum and another with continuous spectrum along with large emittance. The latter is able to generate high-flux betatron X-rays. Such is observed only when the laser self-guiding is extended over 4 mm at a fixed plasma density (4 × 10 18 cm −3 ). Numerical simulation reveals that two bunches of electrons are injected at different stages due to the bubble evolution. The first bunch is injected at the beginning to form a stable quasi-monoenergetic electron beam, whereas the second one is injected later due to the oscillation of the bubble size as a result of the change of the laser spot size during the propagation. Due to the inherent temporal synchronization, this unique electron-photon source can be ideal for pump-probe applications with femtosecond time resolution.S ynchrotron light sources are powerful in generating bright X-rays for a wide range of applications in basic science, medicine, and industry (1). However, these machines are usually large in size and expensive for construction and maintenance and are thus unaffordable to many would-be users. With the advent of tabletop ultrashort and ultraintense lasers, laser plasma acceleration (LPA) proposed by Tajima and Dawson (2) has demonstrated its great potential as a compact accelerator and X-ray source. Significant progress in LPA was made in the last decade (3-11): Well-collimated (approximately millirad) quasi-monoenergetic electron beams were first observed in 2004, and the electron energy above gigaelectronvolts over centimeter-scale acceleration lengths were demonstrated in several laboratories in the last few years.While accelerating longitudinally in the laser wakefield, the electron beams also oscillate transversally (wiggling motion) due to the transverse structure of the wakefield, which emits wellcollimated betatron X-rays (12-14). Among several mechanisms to generate X-ray radiation from laser-plasma interactions (15-20), betatron radiation is straightforward and able to deliver larger X-ray photon fluxes per shot [∼10 8 phs/shot (21)] and higher photon energies [up to gamma rays (22)]. The betatron oscillation frequency is given by ω β = ω p (2γ) −1/2 , where ω p is the plasma frequency and γ is the Lorentz factor of the accelerated electron beam. For large-amplitude betatron oscillations (i.e., a few mi...