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Probably need a better definition of what you want, but:
Locally, Umstead Park has nice trails and whatnot.
Raven Rock State Park is about an hour south (near Lillington), very cool cliffs and hiking
Several other parks with "nature spots"
-There is one on Ten Ten, forgot the name (Crowder?)
-Durant Nature Park
-Yates Mill is really cool.
-Harris Lake Park has a nice peninsula trail
-etc....
White Lake, on the way to Wilmington. And also Wilmington or its beaches - Wrightsville, Carolina...... Or Emerald Point waterpark. Or Kings Dominion in VA.
Aloha Safari Zoo - Home Privately owned zoo in Cameron NC they take rescue animals of all kinds. You can feed most of the animals, is an uplifting environment even though most of the animals came from a rescue situation. They even have a Giraffe named Stretch that you can feed carrots.
http://lifeandscience.org/ Museum of Life and Science in Durham has a bunch of indoor and outdoor fun and animals to explore. Butterfly house, hands on area, train ride.
Lots of good suggestions for local areas. For day trips, in addition to Raven Rock that has been mentioned there is also Hanging Rock, which is right at 100 miles.
I would put Eno River State Park first, in terms of scenery. One of the best waterfalls in the area is on the Few's Ford Trail. Lots of interesting rock formations, cliffs, and some other small waterfalls along the Eno. The Quarry trail is also very good. It's a popular swimming hole. Every trail in this park is interesting.
Second I would have Occoneechee Mountain State Natural Area. The views from the quarry top are the best in the Triangle.
Third, Duke Forest. The Korstian Division has a couple good loops. There's an unexpected cliff on one of the trials.
Umstead is just woods and creeks, nothing special, but there's a lot of it. And it's a great autumn hike.
Further away there's Raven Rock, Cliffs of the Neuse, and the Uwharrie National Forest--which has a number of trails.
I'd also recommend Aloha Safari Zoo. One of our favorite places for a day trip with our toddler.
Also really like the Conservator's Center. It's a big cat sanctuary.
Duke Lemur Center in Duke Forest
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