No. ChromeOS is only designed to work on specific hardware and is mainly for web access. You're also limited to the Chrome Web Store apps. While there are similarities to Android, ChromeOS isn't identical to what you might use on your smartphone.
Android desktops give you more options, such as more apps from the Google Play Store. Plus, you can dual-boot with an existing OS, replace your current system, or boot from an external source. Think of Android desktops as being more flexible and compatible with far more devices.
If you want a quick and easy setup that's regularly updated and may be more secure overall, ChromeOS on a Chromebook is the simplest approach. But, if you want to use an existing device and have more customization options, an Android desktop is best.