Mode-switching supports multilevel operations using a limited number of input methods. In Virtual Reality (VR) head-mounted displays (HMD), common approaches for mode-switching use buttons, controllers, and users' hands. However, they are inefficient and challenging to do with tasks that require both hands (e.g., when users need to use two hands during drawing operations). Using head gestures for mode-switching can be an efficient and cost-effective way, allowing for a more continuous and smooth transition between modes. In this paper, we explore the use of head gestures for mode-switching especially in scenarios when both users' hands are performing tasks. We present a first user study that evaluated eight head gestures that could be suitable for VR HMD with a dual-hand line-drawing task. Results show that move forward, move backward, roll left, and roll right led to better performance and are preferred by participants. A second study integrating these four gestures in Tilt Brush, an open-source painting VR application, is conducted to further explore the applicability of these gestures and derive insights. Results show that Tilt Brush with head gestures allowed users to change modes with ease and led to improved interaction and user experience. The paper ends with a discussion on some design recommendations for using head-based mode-switching in VR HMD.