We present a useful and practical manufacturing technique that enables the structural conversion of delicate as-grown nanostructures to more beneficial and robust thin-film frameworks through controlled mechanical rolling. Functional nanostructures such as carbon nanotubes grown through chemical vapor deposition in a vertically aligned and very loosely packed manner, and thus difficult to manipulate for subsequent uses, can be prepared in an array of thin blades by patterning the growth catalyst layer. They can then be toppled as dominos through precisely controlled mechanical rolling. The nanostructures formulated to horizontally aligned thin films are much more favorable for device applications typically based on thin-film configuration. The proposed technique may broaden the functionality and applicability of as-grown nanostructures by converting them into thin-film frameworks that are easier to handle and more durable and favorable for fabricating thin-film devices for electronics, sensors, and other applications.