The 066 would be a step up from what the 326 HO originally came with. The 066 was the auto trans 1968 350 HO cam, 067 for manual trans. The 066 is a nice upgrade for any 326 I’d say.
All 326 engines came with the 254 cam, 326 HO engines didn’t receive an upgraded cam. High compression heads, a 4-barrel carb and dual exhaust added the extra 35hp over the base 2-barrel 250hp in 1966.
An aftermarket cam is best accompanied by upgraded or at least new valve springs, screw-in 7/16” studs and polylocks. All of this comes with added labor and parts costs in order to end up with a reliable engine.
If you’re keeping the valve springs you have now and the press-in studs I’d leave the stock valvetrain alone and run the 066 cam. The 068 is also a good option but it really will be asking for new valve springs, the 066 would like them too but if you’re not changing springs I’d opt for the 066.
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1964 Tempest Coupe LS3/4L70E/3.42
1964 Le Mans Convertible 421 HO/TH350/2.56
2002 WS6 Convertible LS1/4L60E/3.23
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