The 25-year-old stormed to victory ahead of Canada's Marielle Thompson, with Daniela Maier claiming bronze after Marielle Thompson was bumped down for an infringement.
Naeslund joins Thompson and Jean-Frederic Chapius as the only freestyle skiers to have won Olympic gold, the world championship title and the crystal globe in the event.
Canada have won a medal in all four Games this event has been held, though unlike in 2010, 2014 and 2018, they were unable to stand top of the podium.
Stats Perform picks out some other standout numbers from Thursday's action in Beijing.
7 - Japan's Miho Takagi won her seventh Olympic medal with victory in the women's speed skating 1000m, surpassing China's Wang Meng (six) for the most medals won by an Olympian representing an Asian nation in the Winter Games.
12 - Brittany Bowe claimed bronze in the same event to make it 12 medals for the United States in the women's 1000m, followed by 10 for the Netherlands, who won silver thanks to Jutta Leerdam.
3 - Switzerland's Michelle Gisin became the third athlete to defend her Olympic title in the women's alpine combined after Janica Kostelic in 2002 and 2006 and Maria Hofl-Riesch in 2010 and 2014.
5 - Gisin's team-mate Wendy Holdener won silver for her fifth Olympic medal as Switzerland achieved a gold-silver finish in a women's alpine skiing event at the Winter Games for a third time, previously doing so in the 1956 downhill and 1984 downhill.
7 - Canada prevailed 3-2 winners against the USA in the women's ice hockey final to win their fifth gold medal since its introduction to the Games in 1998. This was the seventh medal in event for both nations, having each made the podium every year the event has been contested.
4 - With two goals on Thursday, Canada's Marie-Phillip Poulin is the only ice hockey player – male or female – to score in four Olympic Games finals, scoring seven times in total across those games.
17 - Anna Shcherbakova and Alexandra Trusova, both 17 years old, won gold and silver respectively in the women's single figure skating, marking the first time that multiple figure skaters under the age of 18 finished on the podium of the event since 1998 when American duo Tara Lipinski (15) and Michelle Kwan (17) won gold and silver respectively.
Thursday's event provided Shiffrin with a chance to redeem herself after crashing out of the giant slalom and slalom, before finishing ninth in the super-G and 18th in the downhill.
But after recording the best time in training on Wednesday, the two-time gold medallist and reigning world champion endured yet more heartbreak on the main run.
She was fifth after the downhill in the two-event competition and well positioned to earn a fourth Winter Olympics medal heading into the slalom run.
However, Shiffrin – famed for her consistency – skied out of the slalom course at the 10th gate at the Yanqing National Alpine Ski Centre.
Switzerland's Michelle Gisin defended her combined crown by finishing more than a second ahead of team-mate Wendy Holdener, while Italy's Federica Brignone took bronze.
Asked by Discovery+ what is not working for her in Beijing, Shiffrin said: "That's the question you want to know and it's what I want to know too.
"I don't really understand what's not working on these races. Especially today.
"Even in the GS and slalom I felt maybe I had too high intensity, I was trying too hard, and I just didn't get into my rhythm first.
"Today I was much more relaxed. Just 'Hey it's slalom, I know how to do slalom, I will take the chance to get into my tempo and start pushing each gate and build it from there.'
"I didn't want to hold back on the run just to make it to the finish – and I wasn't. But I also wasn't going 110 per cent. I was just skiing, and it still didn't work.
"I don't have a really good explanation for it, and you can imagine how annoying that is for me, because I always want to find an explanation. Right now it's just, there isn't one."
Speaking to reporters later on Thursday, Shiffrin went further as she opened up on the hurt of falling short in each event.
"The whole shebang in sport is that you can have preparation, you can have confidence, or maybe you're not fully confident, you can have all of these pieces," she said.
"Sometimes it works, sometimes it doesn't. I have literally no idea why we keep coming back and doing it. Especially after today.
"But I'm going to come back out tomorrow and ski some parallel GS, because I'm that much of an idiot. I don't know why we keep doing it, but making good turns feels amazing.
"And I've been doing that these entire two weeks. I wish there was something to show for it. Right now, I just feel like a joke."
Shiffrin has one final chance to win a medal when competing for the United States in Saturday's mixed team parallel event.
