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This is one of the greatest pieces of Fallout content I've ever experienced, I believe this DLC is on par with some of the greats like Old World Blues for New Vegas.
Right out of the gate, this DLC is a thematic masterclass. The art direction is amazing, and the overall atmosphere and tone of this DLC can only be found in a lesser form through Fallout 3's Point Lookout DLC. The island is amazing, and partially terrifying in Survival, and elements of it such as the dense forest and ruined coastal culture combines with the Fog to create an atmosphere unlike anything else I've ever played. This is the first and only piece of Fallout content that made me want to explore literally everything, even the surrounding ocean of the island. The Fog itself is the single carrying factor of this atmosphere. Watching silhouettes of ghouls and the glowing eyes of predators dance between the muzzle flash of Trapper's rifles in the deep Fog is one of the most scarily exhilarating things in Fallout, competing with Dead Money's entire atmosphere for that spot. Little specks of rural shacks and farms mix with ruined non-quite-developed, almost-urban, coastal towns to break up the overwhelmingly wild environment of the DLC. The music only further amplifies this. This DLC has the greatest fallout soundtrack. Period. Hauntingly beautiful.
Enough praise of the fantastic environment and atmosphere though, since some must be saved for the outstanding story of this DLC as well. For diehard fans of New Vegas (or as I like to call you, close-minded Obsidian dickriders) this DLC's story is perfect for you, since it follows a formula similar to Vegas' story. A personal mystery leads the player character to a 3 conflict between factions, each with their own valid pros AND cons, and each raising an interesting moral conundrum. The factions in this DLC are fantastic, and the ethical questions it raises and philosophical debates it expands upon are great. SPOILERS AHEAD - DiMa is the lifeblood of this DLC's story. His character is fucking fantastic, and he singlehandedly makes the player more willing to side with Acadia. Far Harbor has it's own collection of great characters as well, like the Mariner (seriously such a fantastic character whose story most will miss simply because they missed a dialogue tree during a fetch quest), but the overall community is the town itself is a character on its own. Proud and fiercely independent, but also with its own level of charm, the town is fantastic. This DLC also helps humanize the Children Of Atom, with many of the souls living in the Nucleus just being regular old wastelanders, the only thing separating the two is their deity. This is also contrasted by the High Confessor and his zealots being a more radical and crazed sect of the faith. There's seriously alot to consider with each faction. The final choice is also great, since in reality its a series of choices that gives the player so much agency in the crux of the story. You are given three binary choices in relation to each faction, as opposed to simply just picking one faction. Should you desire, you can detonate the nucleus, turn DiMa into Far Harbor, then flip the kill switch to wipe out every faction, or you can choose to let all three live, and everything in between.
Quick sidenote - Old Longfellow has a lot of potential as a follower. I wish his story was expanded upon, because on the surface he seems very boring, but he does have an interesting backstory and sad motive that you learn about only in his final player dialogue right after you reach max affinity. I've done about 4 playthroughs of this DLC across the past 7 years, and only this most recent time have I even considered him. He needs more incentive to be a companion right away, rather than at the end of his in-game arc. I still very much like him and recommend him as a companion for the DLC playthrough.
Finally, this DLC has some great side quests and side narratives. The best to me is of course the Mariner's story, which through being a series of fetch-quests, is still very engaging because of her personal character. The Vault Murder Mystery and the Dalton storyline are also pretty good fun, and the story with the Heretic for the Children Of Atom is interesting to say the least. This DLC houses some standout locations to explore, like the Cranberry Island Bog, and the Vim factory.
Overall, this DLC is fantastic, a near 10/10 for me, and I highly recommend buying it, even if you despised the base game, as the story and writing will surprise you. This DLC proves Bethesda can know what their doing with this series, and I hope this kind of quality translates over to a Fallout 5 in the future.