Plasma enhanced chemical vapor deposition (PECVD) techniques have been shown to be an efficient method to achieve single-step synthesis of high-quality monolayer graphene (MLG) without the need of active heating. Here we report PECVD-growth of single-crystalline hexagonal bilayer graphene (BLG) flakes and mm-size BLG films with the interlayer twist angle controlled by the growth parameters. The twist angle has been determined by three experimental approaches, including direct measurement of the relative orientation of crystalline edges between two stacked monolayers by scanning electron microscopy, analysis of the twist angle-dependent Raman spectral characteristics, and measurement of the Moiré period with scanning tunneling microscopy. In mm-sized twisted BLG (tBLG) films, the average twist angle can be controlled from 0° to approximately 20°, and the angular spread for a given growth condition can be limited to < 7°. Different work functions between MLG and BLG have been verified by the Kelvin probe force microscopy and ultraviolet photoelectron spectroscopy. Electrical measurements of back-gated field-effect-transistor devices based on small-angle tBLG samples revealed high-quality electric characteristics at 300 K and insulating temperature dependence down to 100 K. This controlled PECVD-growth of tBLG thus provides an efficient approach to investigate the effect of varying Moiré potentials on tBLG.