My opinion (no data yet) is that advancing the cam timing will help improve efficiency in the RPM band where you're trying to get good mileage. There is a risk of piston to valve contact by advancing the cam which can ruin your engine - proceed with caution and know what you're doing. FWIW, when I did this I had PP502's, RC2, 0.681 5th gear, big exhaust and EGR Delete. Cam timing was set wherever VW put it from the factory.
Like I mentioned above, hardware is a supporting factor in this kind of mileage. Ernie Rogers has a couple 70+ MPG tanks in his beetle which has slightly taller tires (~1") and a wing on the back. It does not take a lot of (or any) modifications to get some really good mileage in these cars. The beetle is the least aerodynamic of the ALH powered cars, Jetta wagon is the best.
Driving the speed limit and not being in a hurry are two significant improvements the driver can make.
Not to stick my nose in the air, but 55+ MPG should be relatively straight forward. Set the cruise at the speed limit (65 MPH), fill up 900 miles later.
To improve on that and push into the 60's and 70's MPG takes a lot more work on the drivers part. Managing hills, lights, vehicle speed, wind, a little luck, etc. Think of the car as an energy storage device. You take energy from the fuel in the tank, and turn it into speed and altitude of the car. Anytime that you put more speed in the car than you need and have to slow down using the brakes, you're wasting energy (fuel). Anytime you have to stop at the bottom of a hill, you've wasted the energy that you put into the vehicle getting it to the top of the hill versus being able to carry that momentum through into the next hill or coast it out on the flat after the hill.