In a small bowl, mix together brown sugar, chili powder, salt, paprika, cumin, garlic powder, onion powder, and cayenne pepper. Taste and adjust, if necessary.
Season the chuck roast on all sides with seasoning mixture. Set aside any extra seasoning for later.
Melt butter in a large skillet over medium heat and sear chuck roast on all sides; about 3-5 minutes per side.
Place the seared chuck roast and any juices/brown bits from the pan into a greased 6 quart crockpot. Set aside.
To the hot skillet, add sliced onions, minced garlic, lime juice, and a touch of salt and pepper, and let cook, scrapping up any browned bits, for 5 minutes or until the onions start to soften.
Pour the onions/juices/browned bits over chuck roast in the crock pot, then sprinkle on any remaining seasoning mix.
Cover and cook on LOW for 8 hours (preferred) or HIGH for 4 hours.
Remove the roast from the crockpot, shred the meat with two forks, discarding any extra unwanted fat.
Optional: stir meat back into juices or save the juices in an extra container and use to reheat meat if it’s too dry.