...like here to get individuals' personal impressions...
I'm local, not an american who traveled to the Baltics. Reading your posts i got some contradicting and mixed impressions about your opinion of your future trip. It reads in your profile: "...I admit to being a country counter....", so what's a problem with getting Belarus visa - you get the visa, enter the country, and have one more country in your list. And on your passport. And with a proper visa you can proceed your trip from Belarus any direction, eg to Moscow. You originally didn't intend to visit Belarus, but why do you intend to go to Moscow necessarily from Lithuania?
I'm not against "counting the countries", it's just unusual to read about wide interests of the same person. Either you don't have enough time to satisfy your interests, or the number countries will be fewer. Which one is a priority?
What are the must sees and dos?
The Baltics themselves are neither must sees nor dos. Especially for the person who over the last 41 years have visited over 90 nations - what "adventure & unique experiences" do you expect? Well, there may be some, but you already stressed your rich experience in travels and didn't specify what is, say, "rough idea" or "image" of your trip. Not countries, but your trip. It looks as if you expect to receive the very expert advice, while you yourself are the decent expert in many spheres (given your experience of travels and knowing languages). To me your questions seems rather useless because they look like the questions of a person who is lazy to read the basic info in some basic guidebook. Well, if you've posted some expert question (except that one re visas for americans) it could be difficult to answer, maybe, but it at least would be interesting and worth the challenge.
Regarding transportation. Public transport is good (in local sense), renting a car is recommended for persons who have wide (or just particular) interests, this also is the way that locals do, and not recommended if timeframe is very tight and/or priority is the counting, so to say. To me this all seems quite contradicting situation in everything. And good opportunity to post my reasoning... LOL... Sorry.
What come to mind, having all your questions in mind as a whole one, - get a car, get a list of observation towers and visit them purposefully. You automatically will have the routes and roads ready in your navigation system, or on your print map, or written on the separate list (up to you), you automatically will visit most attractive or picturesque spots of the country (including some in recreation or protected areas), while areas in between will be a "daily-life-thing", and you will be able to check some "alone standing" objects that are scattered everywhere and are always skipped if traveling by public transport. Organizing and implementing that all can count as adventure. Can't say what would be unique, though...