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We've been getting reports of some buyers' PayPal checkouts sporadically ending in an error page that says "Sorry - Your last action could not be completed", rather than being redirected to the proper thank-you page through E-junkie. This is due to a known issue at PayPal's end which they are working to address, as acknowledged by a PayPal rep. here:
https://www.x.com/message/197986#197986

Is there any update to this? My customers, who don't have a paypal account, are experiencing this problem every time they buy my product.

People with Paypal accounts do not experience this problem at all. I've continually reported it to PayPal, but there has been no update. It's been over 3 weeks and I can't drive people to my website with this problem still looming.

There's more discussion about this issue here:
http://www.e-junkie.com/bb/topic/4984

Unfortunately, PayPal still has not confirmed that they've resolved the known issue at their end that's causing this glitch. Since it only seems to affect buyers who pay with a credit card rather than using their PayPal account, you might consider just disabling the card option for all buyers by setting "PayPal Account Optional: OFF" in your PayPal Website Payment Preferences.

You might also consider adding another checkout option for your E-junkie cart; adding Google Checkout would probably be the easiest and most flexible option to add. Buyers who don't have a GC account would simply provide their billing info just like a regular card-based checkout, along with their email address and choice of password. GC will automatically create a GC account for them as part of that checkout, so the next time they use Google Checkout, they can just enter their email and password to use the billing info already stored in that account from the first time. This page explains how to set up Google Checkout:
http://www.e-junkie.com/ej/google-checkout-shopping-cart.htm

We just received word from PayPal today about this issue:

Response (Administrator)
04/12/2011 08:10 AM
Thank you for bringing this issue to our attention. Unfortunately, we have been unsuccessful in recreating the issue. Please confirm that this problem is still occurring. If you are still seeing this issue, please send us additional information to help us identify or reproduce the issue.

PayPal Merchant Technical Services

Reading between the lines there, apparently the issue eventually vanished as mysteriously as it appeared, so all they can say is that it doesn't appear to be happening anymore. We haven't received any reports of this in recent memory, so let's hope that's the end of it.