You can, but you probably have to call up your bank during business hours, wait on hold for a while, and then get given the runaround for a while. PayPal you just push a button and it's done.
In the UK my experience with chargebacks is that they’re very biased towards the company. It’s a drawn-out process during which you get harassed by the company’s anti-chargeback team in to accepting an ex gratia payment etc. you have to supply lots of evidence and when the company provides some poor quality evidence the bank goes “oh well that’s decided then” as if responding was sufficient.
This is true, you have to very persistent with the chargeback route, sometimes only a threat of legal action against the bank will move things forward.