Entangled quantum systems have properties that have fundamentally overthrown the classical worldview. Increasing the complexity of entangled states by expanding their dimensionality allows the implementation of novel fundamental tests of nature, and moreover also enables genuinely new protocols for quantum information processing. Here we present the creation of a (100 × 100)-dimensional entangled quantum system, using spatial modes of photons. For its verification we develop a novel nonlinear criterion which infers entanglement dimensionality of a global state by using only information about its subspace correlations. This allows very practical experimental implementation as well as highly efficient extraction of entanglement dimensionality information. Applications in quantum cryptography and other protocols are very promising.photonic spatial modes | quantum optics | Schmidt rank | entanglement witness Q uantum entanglement of distant particles leads to correlations that cannot be explained in a local realistic way (1-3). To obtain a deeper understanding of entanglement itself, as well as its application in various quantum information tasks, increasing the complexity of entangled systems is important. Essentially, this can be done in two ways. The first method is to increase the number of particles involved in the entanglement (4). The alternative method is to increase the entanglement dimensionality of a system.Here we focus on the latter one, namely on the dimension of the entanglement. The text is structured as follows. After a short review of properties and previous experiments, we present a unique method to verify high-dimensional entanglement. Then we show how we experimentally create our high-dimensional two-photon entangled state. We analyze this state with our method and verify a 100 × 100-dimensional entangled quantum system. We conclude with a short outlook to potential future investigations.High-dimensional entanglement provides a higher information density than conventional two-dimensional (qubit) entangled states, which has important advantages in quantum communication. First, it can be used to increase the channel capacity via superdense coding (5). Second, high-dimensional entanglement enables the implementation of quantum communication tasks in regimes where mere qubit entanglement does not suffice. This involves situations with a high level of noise from the environment (6, 7), or quantum cryptographic systems where an eavesdropper has manipulated the random number generator involved (8). Moreover, the entangled dimensions of the whole Hilbert space also play a very interesting role in quantum computation: high-dimensional systems can be used to simplify the implementation of quantum logic (9). Furthermore, it has been found recently (10) that any continuous measure of entanglement (such as concurrence, entanglement of formation, or negativity) can be very small, while the quantum system still permits an exponential computation speedup over classical machines. This is not the case for the dim...