Before heading out to find these armor pieces, you must first prepare your Power Armor suit. The Freefall Armor is located on one of the top floors of the Mass Fusion Building. Since there is no direct path to reach this floor, players must jump to this upper level instead by using a suit of Power Armor equipped with a jetpack. Jetpacks can be crafted as a torso mod in the Power Armor workbench, but require Rank 4 in both the Science! and Armorer perk abilities. You may also want to bring along some Ultra Jet, Buffjet, or Nuka Cola Quantum as well.
Put on your jetpack-enabled Power Armor suit, and Fast Travel to the Mass Fusion Building, north of Goodneighbor near the Old Corner Bookstore. Enter the building, and head up the elevator to the fifth floor. Ride the next elevator up as far as it can go. Head forward through the corridor until you reach the open area in the center of the building. Here you will see a sort of jumping puzzle, composed of broken platforms for each floor overlooking an open center chamber.
Note that you need to be pretty far along in the main story to use the elevator. If you don’t have elevator access, walk up the stairs to the second floor, and unlock a door in a hallway at the other end of the walkway. Keep heading up through the rooms to the area with the glass ceiling. Look for a hole in the ceiling, and jump up into a small room. This room contains an Expert locked door. Level up your Lockpicking perk to open it to reach the same jumping puzzle.
Start jumping up along each platform to scale your way towards the top level. The jetpack height is limited and drains Action Points for each jump, so you will likely only be able to scale up one floor at a time. Continue scaling upward until you reach the highest platform where you can boost through a hole in the floor above. From the balcony, you should be able to see a few small rooms tucked higher up along the walls. The Freefall Armor is found in one of these the upper rooms.
Make sure to quicksave before attempting to scale any higher. The goal is to boost up along the wall in small increments, in order to reach the nearest room across from the balcony. Just before you begin hopping up the wall, consume some Buffout as well as Nuka Cola Quantum to temporarily slow down time and increase your AP, or simply take some Ultra Jet for the same effects. Now, hop onto the balcony railing, and jump toward the corner of the wall. Tap the jump button to boost up in small bursts, until you reach a small debris filled room. Take a brief moment to quicksave in this room, and make sure to snag the Fusion Core off the nearby desk as well.
From the small room, jump across the gap towards the opposite corner and repeat the same process. Boost your way up along the corner, sticking yourself to the wall as you ascend. There is a small office a short distance up, which should be a bit easier to reach than the first room. Here you will find a locked safe on the floor that contains the Freefall Armor, along with various types of ammo. Pick the novice lock on the safe to claim the rare loot. Also, make sure to grab the holotape from the nearby computer terminal before you leave.
Now that you have this awesome new armor, feel free to leap from new heights without Power Armor or fear of fall damage. For more Fallout 4 features, check out our Fallout 4 Walkthrough and Guide.