file lookups work on the controller, not the target hosts. So you’d be stuck doing a ansible.builtin.stat on those paths first, then some magic jinja expressions on the results. It gets messy, much messier than what you’re already doing.
But, unless you’re the creating a service yourself - and I mean the whole service, not just the systemd unit file - this is not the way to go. Systemd provides a mechanism for the sysadmin to override and/or add to the settings in a vendor- or distro-provided service unit. You should consider putting your overrides in /etc/systemd/system/chronyd.service.d/ and leaving the upstream service unit file(s) alone. This also preserves your mods and avoids conflicts across chronyd updates.