Used to be able to drop it in Chrome but I don't think that works anymore. However I think if you start playing it full screen then goto Chrome and cast a screen then you can select it (at least in Windows).
What I do with my laptop is use it like an HTPC. Connect if via HDMI and use a wireless keyboard w/ trackpad. (Logitech K400 is like 30 bucks). This typically provides a better experience all around. Take it a step further an get Kodi and its a pretty good HTPC experience all around if you have a large movie collection.
Feature to cast from vlc to chromecast is only available in vlc nighly version, so first you need to install nightly version of vlc and then you can follow steps from below site to setup vlc to stream from vlc to tv via chromecast https://wildtricks.com/vlc-chromecast-setup-tv/
Seems to have a basic level of functionality now that the good people over at VLC released 3.0. You'll have to go to Menu>Playback>Renderer>Chromecast. Note that subtitles don't seem to be supported yet.