From November 1999 through July 2000, a broadband seismic experiment was carried out at Popocatépetl Volcano to record seismic activity over a wide period range (0.04–100 s). We present an overview of the seismicity recorded during this experiment and discuss results of analyses of long-period (LP) and very-long-period (VLP) seismic signals recorded at stations nearest to the crater over a four-month interval December 1999–March 2000. Three families of LP signals (Types-I, II, and III) are identified based on distinctive waveform features observed periods shorter than 1 s, periods longer than 15 s, and within the period range 0.5–2.5 s. Type-I LP events have impulsive first arrivals and exhibit a characteristic harmonic wave train with dominant periods in the 1.4–1.9 s range during the first 10 s of signal. These events are also associated with a remarkable VLP wavelet with period near 30 s. Type-II LP events represent pairs of events occurring in rapid succession and whose signatures are superimposed. These are typically marked by slowly emergent first arrivals and by a characteristic VLP wave train with dominant period near 30 s, made of two successive wavelets whose shapes are quasi-identical to those of the VLP wavelets associated with Type-I events. Type-III LP events represent the most energetic signals observed during our experiment. These have an emergent first arrival and display a harmonic signature with dominant period near 1.1 s. They are dominated by periods in the 0.25–0.35 s band and contain no significant energy at periods longer than 15 s. Hypocentral locations of the three types of LP events obtained from phase picks point to shallow seismic sources clustered at depths shallower than 2 km below the crater floor. Observed variations in volcanic eruptive activity correlate with defined LP families. Most of the observed seismicity consists of Type-I events that occur in association with 1–3-min-long degassing bursts (“exhalations”). Eruptive activity increased in intensity in February, coinciding with an increasing occurrence of Type-II LP events. Type-III events were first observed at the end of February and during March, in coincidence with the formation of a new lava dome. Vulcanian eruptions occurred in April and May. These events typically exhibit broadband signatures extending over the full period range of the sensors and lasting 30–80 min.