Third-party themes can’t be uploaded on WordPress.com sites, whether or not you purchase a Value Bundle.
If you absolutely need a third-party theme that WordPress.com doesn’t offer you may want to look into a self-hosted WordPress installation, using your own hosting. Only self-hosted sites can upload themes. You can learn more about the differences between WordPress.com and WordPress.org here:
You may also want to browse the WordPress.com theme directory using the advanced filters, if you haven’t already. Just click “Find a theme” and choose from some of the options in each filter to help you find what you’re looking for: