Abstract-Imaging controlled molecules with ultrashort xray pulses from free-electron lasers enables the recording of "molecular movies", i.e., snapshots of molecules at work, with spatial (picometer) and temporal (femtosecond) atomic resolution.Hard-x-ray free-electron lasers (FELs) provide femtosecond-duration pulses of x-rays with unprecedented brilliance [1], [2]. These enable the study of ultrafast chemical dynamics of isolated molecules in the gas phase using diffractive-imaging methods [3]- [7]. We exploit various imaging approaches to understand the intrinsic molecular structure and function, which is at the very heart of the chemical and molecular sciences.Experiments that allow for the creation of structurally pure samples and, subsequently, for the investigation of their intrinsic molecular dynamics and chemical function have developed tremendously over the last few decades, although "there's plenty of room at the bottom" -for better control as well as for further applications. We detail the use of inhomogeneous electric fields for the manipulation of neutral molecules in the gas-phase, i.e., for the separation of complex molecules according to size, structural isomer, and quantum state [8]- [12]. These quantum-state-selected samples allow for very strong degrees of alignment and orientation [9], [13]- [17]. The produced ensembles of structurally sorted and fixed-inspace molecules are well-suited for imaging experiments, as the availability of many identical molecules in the camera's frame of reference allows for direct, experimental averaging of the recorded signal until it is above noise.We have performed a number of imaging experiments at the Linac Coherent Light Source (LCLS) at SLAC [2] and the Free-Electron Laser in Hamburg (FLASH) at DESY [18]. These include the direct x-ray-diffractive imaging of aligned isolated gas-phase molecules [19], [20] and photoelectronholography approaches, which are implemented as imaging of molecular-frame photoelectron angular distributions (MF-PAD) [21]-[23]. In these first benchmark imaging experiments, we have exploited cold molecular beams from state-of-theart pulsed valves. These beams were further purified using the electric deflector [24], which spatially disperses the beam according to the molecules' quantum states and separates the molecules from the atomic seed gas. The quantum-state selected samples were laser aligned or mixed-field oriented using nanosecond-pulsed Nd:YAG lasers or stretched pulses from amplified Ti:Sapphire laser systems. The latter allows to generate strong alignment and orientation at full FEL repetition rates [15], [25].