Heterografted molecular bottlebrushes (MBBs) with side chains composed of poly(n-butyl acrylate) (PnBA) and pH-responsive poly(2-(N,N-diethylamino)ethyl methacrylate) (PDEAEMA, pKa = 7.4) have been shown to be efficient, robust, and responsive emulsifiers. However, it remains unknown how they respond to external stimuli at interfaces. In this work, the shape-changing behavior of six hetero- and homografted MBBs at air-water interfaces in response to pH changes and lateral compression was investigated using a Langmuir-Blodgett trough and atomic force microscopy. At a surface pressure of 0.5 mN m-1, PDEAEMA-containing MBBs showed no worm-globule transitions when the pH was increased from 4.0 to 10.0, at which PDEAEMA becomes insoluble in water. Upon lateral compression at pH 4.0, MBBs with a mole fraction of PDEAEMA side chains (xPDEAEMA) < 0.50 underwent pronounced worm-globule shape transitions; there was an increasing tendency for bottlebrushes to become connected with increasing xPDEAEMA. At xPDEAEMA = 0.76, the molecules remained wormlike even at high compression. These observations were presumably caused by the increased electrostatic repulsion between protonated PDEAEMA side chains in the subphase with increasing xPDEAEMA, hindering the shape change. At pH 10.0, MBBs with xPDEAEMA < 0.50 showed a lower tendency to change their wormlike morphologies upon compression than at pH 4.0. No shape transition was observed when xPDEAEMA > 0.50, attributed to the relatively high affinity toward water and the rigidity of PDEAEMA. This study revealed the shape-changing behavior of amphiphilic pH-responsive MBBs at air-water interfaces, which could be useful for future design of multicomponent MBBs for potential applications.