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This paper reports recently completed structural dynamics experimental activities with new ultralightweight and inflatable space structures (a.k.a., "Gossamer" spacecraft) at NASA Langley Research Center, NASA Marshall Space Flight Center, and NASA Goddard Space Flight Center. Nine aspects of this work are covered: 1) inflated, rigidized tubes, 2) active control experiments, 3) photogrammetry, 4) laser vibrometry, 5) modal tests of inflatable structures, 6) in-vacuum modal tests, 7) tensioned membranes, 8) deployment tests, and 9) flight experiment support. Structural dynamics will play a major role in the design and eventual in-space deployment and performance of Gossamer spacecraft. Experimental research and development such as this is required to validate new analysis methods. The activities discussed in the paper are pathfinder accomplishments, conducted on unique components and prototypes of future spacecraft systems.